Publications Repository - Helmholtz-Zentrum Dresden-Rossendorf

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41396 Publications

Synthesis, Structures and Photophysical Properties of Tetra- and Hexanuclear Zinc Complexes Supported by Tridentate Schiff Base Ligands

Severin, T.; Karabtsova, V.; Börner, M.; Weiske, H.; Kuc, A. B.; Kersting, B.

The synthesis, structure and photophysical properties of two polynuclear zinc complexes, namely Zn6 L2 (μ3 -OH)2 (OAc)8 ] (1) and [Zn4 L4 (μ2 -OH)2 * emission. Other biologically relevant ions, i.e., Na+, K+, Mg2+, Ca2+, Mn2+, Fe2+, Co2+, Ni2+ and Cu2+, did not give rise to a fluorescence enhancement.

Permalink: https://www.hzdr.de/publications/Publ-37316
Publ.-Id: 37316


Measurements of radioactive 60Fe and 244Pu deposits on Earth and Moon

Wallner, A.

Earth is exposed to nearby cosmic events. The solar system moves through the
interstellar medium and collects interstellar dust particles that contain unique
signatures of ongoing nucleosynthesis in nearby supernovae or rare cosmic
explosions. Such particles may accumulate over million years in deep-ocean
archives and in lunar soil, imprinting isotopic fingerprints of specific interstellar
radionuclides in the geological record. The most prominent radionuclides are
60Fe (t1/2 = 2.6 Myr) and 244Pu (81 Myr). Both do not exist naturally on Earth.
They can be measured with high sensitivity via accelerator mass spectrometry
(AMS). Indeed, both nuclides have been found on Earth and 60Fe also on the
Moon.
AMS measurements of 60Fe from terrestrial and lunar archives demonstrate
a clear exposure of Earth to recent (<10 Myr) cosmic explosions, suggesting
close-by supernova activity ∼2–3 and ∼7 million years ago. In addition, recent
detection of interstellar 244Pu, exclusively produced by the rapid neutron capture
(r-)process, allows to link supernovae and r-process. This latter process is far
from being fully understood. Interstellar 244Pu can place constraints on r-process
frequency and production yields over the last few 100 Myr. The measured
244Pu influx was found lower than expected if supernovae dominate r-process
nucleosynthesis, implying contributions from additional sources.
In this chapter, the journey of such radionuclides is followed, after their
production in massive stars or compact objects, from the interstellar medium
to their incorporation in geological archives, resulting finally in the detection of
a few atoms via direct atom counting. These experimental results provide unique
insights into recent and nearby nucleosynthesis events.

Keywords: interstellar medium; AcceleratorMass Spectrometry; radionuclides; supernovae; r process; lunar samples

  • Book chapter
    Isao Tanihata, Hiroshi Toki, Toshitaka Kajino: Handbook of Nuclear Physics, Singapore: Springer, 2023, 978-981-15-8818-1, 1-47
    DOI: 10.1007/978-981-15-8818-1_94-1

Permalink: https://www.hzdr.de/publications/Publ-37315
Publ.-Id: 37315


Atom Counting with Accelerator Mass Spectrometry

Kutschera, W.; Timothy Jull, A. J.; Paul, M.; Wallner, A.

Accelerator mass spectrometry (AMS) was born in the late 1970s when it was realized at nuclear physics laboratories that the accelerator systems can be used as a sensitive mass spectrometer to measure ultra-low traces of long-lived radioisotopes. It soon became possible to measure radioisotope-to-stable isotope ratios in the range from 10−12 to 10−16 by counting the radioisotope ions "atom by atom’’ and comparing the count rate with ion currents of stable isotopes (1.6 A = 1x10^13 singly-charged ions/sec). It turned out that electrostatic tandem accelerators are best suited for this, and there are now world-wide about 160 AMS facilities based on this principle. The current review will present the history, technological developments and research areas of AMS through the 45 years since its discovery. Many different fields are touched by AMS measurements, including (alphabetically) archaeology, astrophysics, atmospheric science, biology, climatology, cosmic-ray physics, environmental physics, forensic science, glaciology, geophormology, hydrology, ice core research, meteoritics, nuclear physics, oceanography, particle physics - and more. Since it is virtually impossible to discuss all fields in detail in this review, only some specific fields with recent advances will be highlighted in more detail. For the others, an effort has been made to provide relevant references for in-depth studies of the respective fields.

Keywords: accelerator mass spectrometry; Long-lived Radioisotopes; Technical Aspects of AMS; The wide-ranging research areas of AMS; Nuclear Physics and Astrophysics

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  • Secondary publication expected

Permalink: https://www.hzdr.de/publications/Publ-37314
Publ.-Id: 37314


Deep-Sea and Lunar Radioisotopes from Nearby Astrophysical Explosions

Fields, B. D.; Wallner, A.

Earth is exposed to nearby cosmic events. The solar system moves through the interstellar medium and collects interstellar dust particles that contain unique signatures of ongoing nucleosynthesis in nearby supernovae or rare cosmic explosions. Such particles may accumulate over million years in deep-ocean archives and in lunar soil, imprinting isotopic fingerprints of specific interstellar radionuclides in the geological record. The most prominent radionuclides are 60Fe (t1/2=2.6 Myr) and 244Pu (81 Myr). Both do not exist naturally on Earth. They can be measured with high sensitivity via accelerator mass spectrometry (AMS). Indeed, both nuclides have been found on Earth or the Moon.
AMS measurements of 60Fe from terrestrial and lunar archives demonstrate a clear exposure of Earth to recent (<10 Myr) cosmic explosions, suggesting close-by supernova activity ~2–3 and ~6 million years ago. In addition, recent detection of interstellar 244Pu, exclusively produced by the rapid neutron capture (r-)process, allows to link supernovae and r-process. This latter process is far from being fully understood. Interstellar 244Pu can place constraints on r-process frequency and production yields over the last few 100 Myr. The measured 244Pu influx was found lower than expected if supernovae dominate r-process nucleosynthesis, implying contributions from additional sources.
In this chapter we follow the journey of such radionuclides after production in massive stars or compact objects, from the interstellar medium to their incorporation in geological archives, resulting finally in the detection of a few atoms via a direct atom counting. These experimental results provide unique insights into recent and nearby nucleosynthesis events.

Keywords: supernovae; nucleosynthesis; r-process; accelerator mass spectrometry

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37312
Publ.-Id: 37312


3D Magnonic Conduits by Direct Write Nanofabrication

Lamb-Camarena, S.; Porrati, F.; Kuprava, A.; Wang, Q.; Urbánek, M.; Barth, S.; Makarov, D.; Huth, M.; Dobrovolskiy, O. V.

Magnonics is a rapidly developing domain of nanomagnetism, with application potential in information processing systems. Realisation of this potential and miniaturisation of magnonic
circuits requires their extension into the third dimension. However, so far magnonic conduits are largely limited to thin films and 2D structures. Here, we introduce 3D magnonic nanoconduits fabricated by the direct write technique of focused electron beam induced deposition (FEBID). We use Brillouin light scattering (BLS) spectroscopy to demonstrate significant qualitative differences in spatially resolved spin-wave resonances of 2D and 3D nanostructures, which originates from the geometrically induced nonuniformity of the internal field. This work demonstrates the capability of FEBID as an additive manufacturing technique to produce magnetic 3D nanoarchitectures and presents the first report of BLS spectroscopy characterisation of FEBID conduits.

Keywords: nanomagnetism; 3D nanostructures; spin waves

Permalink: https://www.hzdr.de/publications/Publ-37311
Publ.-Id: 37311


Overcoming radioresistance with the hypoxia-activated prodrug CP-506: A pre-clinical study of local tumour control probability

Yaromina, A.; Koi, L.; Schuitmaker, L.; van der Wiel, A. M.-M. A.; Dubois, L. J.; Krause, M.; Lambin, P.

Background and purpose: Tumour hypoxia is an established radioresistance factor. A novel hypoxia-activated prodrug CP-506 has been proven to selectively target hypoxic tumour cells and to cause anti-tumour activity. The current study investigates whether CP-506 improves outcome of radiotherapy in vivo.
Materials and methods: Mice bearing FaDu and UT-SCC-5 xenografts were randomized to receive 5 daily injections of CP-506/vehicle followed by single dose (SD) irradiation. In addition, CP-506 was combined once per week with fractionated irradiation (30 fractions/6 weeks). Animals were followed-up to score all recurrences. In parallel, tumours were harvested to evaluate pimonidazole hypoxia, DNA damage (cH2AX), expression of oxidoreductases.
Results: CP-506 treatment significantly increased local control rate after SD in FaDu, 62% vs. 27% (p = 0.024). In UT-SCC-5, this effect was not curative and only marginally significant. CP-506 induced significant DNA damage in FaDu (p = 0.009) but not in UT- SCC-5. Hypoxic volume (HV) was significantly smaller (p = 0.038) after pretreatment with CP-506 as compared to vehicle in FaDu but not in less responsive UT-SCC-5. Adding CP-506 to fractionated radiotherapy in FaDu did not result in significant benefit.
Conclusion: The results support the use of CP-506 in combination with radiation in particular using hypofractionation schedules in hypoxic tumours. The magnitude of effect depends on the tumour model, therefore it is expected that applying appropriate patient stratification strategy will further enhance the benefit of CP-506 treatment for cancer patients. A phase I-IIA clinical trial of CP-506 in monotherapy or in combination with carboplatin or a checkpoint inhibitor has been approved (NCT04954599).

Keywords: Hypoxia-activated prodrug CP-506; Radiotherapy; Hypoxia; Xenografts; Local control

Permalink: https://www.hzdr.de/publications/Publ-37309
Publ.-Id: 37309


Ge–Cu-Complexes Ph(pyO)Ge(μ²-pyO)₂CuCl and PhGe(μ²-pyO)₄CuCl - Representatives of Cu(I)→Ge(IV) and Cu(II)→Ge(IV) Dative Bond Systems

Wagler, J.; Gericke, R.

Phenylgermaniumpyridine-2-olate PhGe(pyO)₃ (compound 1Ge) and CuCl react with the formation of the heteronuclear complex Ph(pyO)Ge(μ²-pyO)₂CuCl (2Ge’) rather than forming the expected compound PhGe(μ²-pyO)₃CuCl (2Ge). Single-point calculations (at the B2T-PLYP level) of the optimized molecular structures confirmed the relative stability of isomer 2Ge’ over 2Ge and, for the related silicon congeners, the relative stability of 2Si over 2Si’. Decomposition of a solution of 2Ge’ upon access to air provided access to some crystals of the copper(II) compound PhGe(μ²-pyO)₄CuCl (3Ge). Compounds 2Ge’ and 3Ge were characterized by single-crystal X-ray diffraction analyses, and the Ge–Cu bonds in these compounds were analyzed with the aid of quantum chemical calculations, e.g., Natural Bond Orbital analyses (NBO), Non-Covalent Interactions descriptor (NCI), and topology of the electron density at bond critical point using Quantum Theory of Atoms-In-Molecules (QTAIM) in conjunction with the related silicon compounds PhSi(μ²-pyO)₃CuCl (2Si), PhSi(μ²-pyO)₄CuCl (3Si), as well as the potential isomers Ph(pyO)Si(μ²-pyO)₂CuCl (2Si’) and PhGe(μ²-pyO)₃CuCl (2Ge). Pronounced Cu→Ge (over Cu→Si) lone pair donation was found for the Cu(I) compounds, whereas in Cu(II) compounds 3Si and 3Ge, this σ-donation is less pronounced and only marginally enhanced in 3Ge over 3Si.

Keywords: atoms-in-molecules; copper; dimetallic complexes; NLMO; single-crystal X-ray diffraction analyses

Permalink: https://www.hzdr.de/publications/Publ-37307
Publ.-Id: 37307


All-electrical operation of a Curie-switch at room temperature

Iurchuk, V.; Kozlov, O.; Sorokin, S.; Zhou, S.; Lindner, J.; Reshetniak, S.; Kravets, A.; Polishchuk, D.; Korenivski, V.

We present all-electrical operation of a Fe$_x$Cr$_{1-x}$-based Curie switch at room temperature. More specifically, we study the current-induced thermally-driven transition from ferromagnetic to antiferromagnetic Ruderman-Kittel-Kasuya-Yosida (RKKY) indirect coupling in a Fe/Cr/Fe$_{17.5}$Cr$_{82.5}$/Cr/Fe multilayer. Magnetometry measurements at different temperatures show that the transition from the ferromagnetic to the antiferromagnetic coupling at zero field is observed at $\sim$325K. Analytical modelling confirms that the observed temperature-dependent transition from indirect ferromagnetic to indirect antiferromangetic interlayer exchange coupling originates from the modification of the effective interlayer exchange constant through the ferromagnetic-to-paramagnetic transition in the Fe$_{17.5}$Cr$_{82.5}$ spacer with minor contributions from the thermally-driven variations of the magnetization and magnetic anisotropy of the Fe layers. Room-temperature current-in-plane magnetotransport measurements on the patterned Fe/Cr/Fe$_{17.5}$Cr$_{82.5}$/Cr/Fe strips show the transition from the 'low-resistance' parallel to the 'high-resistance' antiparallel remanent magnetization configuration, upon increased probing current density. Quantitative comparison of the switching fields, obtained by magnetometry and magnetotransport, confirms that the Joule heating is the main mechanism responsible for the observed current-induced resistive switching.

Keywords: RKKY coupling; Interlayer exchange; Spin valve; Magnetoresistance; Joule heating

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Permalink: https://www.hzdr.de/publications/Publ-37306
Publ.-Id: 37306


Data publication: The DRESDEN PLATFORM – A Research Hub for Ultra-high Dose Rate Radiobiology

Metzkes-Ng, J.; Brack, F.-E.; Kroll, F.; Bernert, C.; Bock, S.; Bodenstein, E.; Brand, M.; Cowan, T.; Gebhardt, R.; Hans, S.; Helbig, U.; Horst, F. E.; Jansen, J.; Kraft, S.; Krause, M.; Leßmann, E.; Löck, S.; Pawelke, J.; Püschel, T.; Reimold, M.; Rehwald, M.; Richter, C.; Schlenvoigt, H.-P.; Schramm, U.; Schürer, M.; Seco, J.; Szabó, E. R.; Umlandt, M. E. P.; Zeil, K.; Ziegler, T.; Beyreuther, E.

Source data, scripts and parts of figures to generate the figures in publication

Keywords: Laser-Plasma Acceleration; FLASH; Radiobiology; Laser-driven proton acceleration; TNSA; UHDR; Ultra-high dose rate; Cancer; Radiotherapy

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Permalink: https://www.hzdr.de/publications/Publ-37304
Publ.-Id: 37304


The DRESDEN PLATFORM – A Research Hub for Ultra-high Dose Rate Radiobiology

Metzkes-Ng, J.; Brack, F.-E.; Kroll, F.; Bernert, C.; Bock, S.; Bodenstein, E.; Brand, M.; Cowan, T.; Gebhardt, R.; Hans, S.; Helbig, U.; Horst, F. E.; Jansen, J.; Kraft, S.; Krause, M.; Leßmann, E.; Löck, S.; Pawelke, J.; Püschel, T.; Reimold, M.; Rehwald, M.; Richter, C.; Schlenvoigt, H.-P.; Schramm, U.; Schürer, M.; Seco, J.; Szabó, E. R.; Umlandt, M. E. P.; Zeil, K.; Ziegler, T.; Beyreuther, E.

The recently observed FLASH effect provides normal tissue protection at a similar tumor treatment efficacy via ultra-high dose rate (UHDR) irradiation and promises great benefits for radiotherapy patients. Dedicated studies are now necessary to define a robust set of dose application parameters for FLASH radiotherapy and to identify underlying mechanisms. These studies require particle accelerators with variable temporal dose application characteristics for numerous radiation qualities, equipped for preclinical radiobiological research. Here we present the DRESDEN PLATFORM, a research hub for ultra-high dose rate radiobiology. By uniting clinical and research accelerators with radiobiology infrastructure and know-how, the DRESDEN PLATFORM offers a unique environment for studying the FLASH effect. We introduce its experimental capabilities and qualify the platform for systematic investigation of FLASH by presenting results from a concerted in vivo radiobiology study with zebrafish embryos. The comparative pre-clinical study was conducted across three accelerator facilities, including an advanced laser-driven proton source applied for FLASH-relevant in vivo irradiations for the first time. The data show a protective effect of UHDR irradiation up to 10^5 Gy/s and suggests consistency of the protective effect even at escalated dose rates of 10^9 Gy/s. With
the first clinical FLASH studies underway, research facilities like the DRESDEN PLATFORM, addressing the open questions surrounding FLASH, are essential to accelerate FLASH’s translation into clinical practice.

Keywords: Laser-Plasma Acceleration; FLASH; Radiobiology; Laser-driven proton acceleration; TNSA; UHDR; Ultra-high dose rate; Cancer; Radiotherapy

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Permalink: https://www.hzdr.de/publications/Publ-37303
Publ.-Id: 37303


Microstructural characterization of reactor pressure vessel steels

Lai, L.; Chekhonin, P.; Akhmadaliev, S.; Brandenburg, J.-E.; Bergner, F.

Ion irradiation is a promising tool to emulate neutron-irradiation effects on reactor pressure vessel (RPV) steels, especially in the situation of limited availability of suitable neu-tron-irradiated material. This approach requires the consideration of ion-neutron transferability issues, which are addressed in the present study by comparing the effect of ions with neu-tron-irradiation effects reported for the same materials. The first part of the study covers a com-prehensive characterization, based on dedicated electron microscopy techniques, of the selected unirradiated RPV materials, namely a base metal and a weld. The results obtained for the grain size, dislocation density and precipitates are put in context in terms of hardening contributions and sink strength. The second part is focused on the depth-dependent characterization of the dislocation loops formed in ion-irradiated samples. This work is based on scanning transmission electron microscopy applied to cross-sectional samples prepared by the focused ion beam tech-nique. A band-like arrangement of loops is observed in the depths range close to the peak of in-jected interstitials. Two levels of displacement damage, 0.1 and 1 dpa (displacements per atom), as well as post-irradiation annealed conditions are included for both RPV materials. Compared with neutron irradiation, ion irradiation creates a similar average size but a higher number density of loops presumably due to the higher dose rate during ion irradiation.

Keywords: reactor pressure vessel steels; microstructural characterization; ion irradiation; transmission electron microscope; dislocation loop

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Permalink: https://www.hzdr.de/publications/Publ-37302
Publ.-Id: 37302


Bottom-Up Synthesis of Crystalline Covalent Organic Framework Nanosheets, Nanotubes, and Kippah Vesicles: An Odd–Even Effect Induction

Koner, K.; Sadhukhan, A.; Karak, S.; Sekhar Sasmal, H.; Ogaeri, Y.; Nishiyama, Y.; Zhao, S.; Polozij, M.; Kuc, A. B.; Heine, T.; Banerjee, R.

Few-layer organic nanosheets are becoming increasingly attractive as two-dimensional (2D) materials due to their precise atomic connectivity and tailor-made pores. However, most strategies for synthesizing nanosheets rely on surface-assisted methods or top-down exfoliation of stacked materials. A bottom-up approach with well-designed building blocks would be the convenient pathway to achieve the bulk-scale synthesis of 2D nanosheets with uniform size and crystallinity. Herein, we have synthesized crystalline covalent organic framework nanosheets (CONs) by reacting tetratopic thianthrene tetraaldehyde (THT) and aliphatic diamines. The bent geometry of thianthrene in THT retards the out-of-plane stacking, while the flexible diamines introduce dynamic characteristics into the framework, facilitating nanosheet formation. Successful isoreticulation with five diamines with two to six carbon chain lengths generalizes the design strategy. Microscopic imaging reveals that the odd and even diamine-based CONs transmute to different nanostructures, such as nanotubes and hollow spheres. The single-crystal X-ray diffraction structure of repeating units indicates that the odd–even linker units of diamines introduce irregular–regular curvature in the backbone, aiding such dimensionality conversion. Theoretical calculations shed more light on nanosheet stacking and rolling behavior with respect to the odd–even effects.

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  • Secondary publication expected from 20.06.2024

Permalink: https://www.hzdr.de/publications/Publ-37301
Publ.-Id: 37301


Microfabrication Approaches on Magnetic Shape Memory Films

Kar, S.; Nielsch, K.; Fähler, S.; Reith, H.

Magnetic shape memory alloys are emerging multifunctional materials that enable applications
like high-stroke actuation, solid-state refrigeration, and energy harvesting of waste heat. Thin
films of these alloys promise integration in microsystems to exploit their multifunctional
properties at the microscale. However, the microfabrication process of these Heusler alloys is
difficult. Here, we investigate different etching techniques for the microfabrication of epitaxial
Ni-Mn-Ga films, explain the encountered challenges, and demonstrate ways to overcome them.
Our results show that wet chemical etching is suitable for large patterned structures, while
reactive ion etching of Ni-Mn-Ga films is unsuitable due to redeposition. For patterning
structures below 10 μm with clean and sharp edges, the best results are obtained by ion-beam
etching with adjusted sample-stage tilt. Finally, we demonstrate a microfabrication process
using Si microtechnology to fabricate partially free-standing structures. Our findings give
guidelines for the fabrication and integration of these smart materials in Si-based microsystems.

Keywords: magnetic shape memory alloys; epitaxial films; microfabrication; redeposition; ion-beam etching; freestanding structures

Permalink: https://www.hzdr.de/publications/Publ-37300
Publ.-Id: 37300


Underground hyperspectral outcrop scanning for automated mine-face mapping — the Lithium deposit of Zinnwald/Cínovec

Kirsch, M.; Mavroudi, M.; Thiele, S. T.; Lorenz, S.; Tusa, L.; Booysen, R.; Herrmann, E.; Fatihi, A.; Möckel, R.; Dittrich, T.; Gloaguen, R.

The inherent complexity of underground mining requires highly selective ore extraction and adaptive mine planning. Repeated geological face mapping and re-interpretation throughout mine life is therefore routine in underground mines. Hyperspectral imaging has successfully been applied to enhance geological mapping in surface mining environments but remains a largely unexplored opportunity in underground operations due to challenges associated with illumination, wet surfaces, and data corrections. In this study, we propose a workflow that paves the way for the operational use of hyperspectral imaging in active underground mines. In a laboratory setup, we evaluated different hyperspectral sensors and lighting setups as well as the effect of surface moisture. We then acquired hyperspectral data in an underground mine of the Zinnwald/Cínovec Sn-W-Li greisen-type deposit in Germany. These data were corrected for illumination effects, back-projected into 3-D and then used to map mineral abundance and estimate lithium content across the mine face. We validated the results with handheld laser-induced breakdown spectroscopy. Despite remaining challenges, we hope this study will help establish hyperspectral sensors in the extractive industry as a means to increase the volume and efficiency of raw material supply, advance digitalisation, and reduce the environmental footprint and other risks associated with underground mining.

Keywords: hyperspectral; underground mining; point cloud; lithium; mineral mapping

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  • Open Access Logo The Photogrammetric Record 38(2023)183, 408-429
    Online First (2023) DOI: 10.1111/phor.12457

Permalink: https://www.hzdr.de/publications/Publ-37299
Publ.-Id: 37299


Codes, Models and Data for Learning locally dominant force balances in active particle systems

Sturm, D.; Maddu, S.; Sbalzarini, I. F.

Here, we provide all the codes, models and datasets for the submission "Learning locally dominant force balances in active particle systems".

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Permalink: https://www.hzdr.de/publications/Publ-37298
Publ.-Id: 37298


Energy Price as an Input to Fuzzy Wastewater Level Control in Pump Storage Operation

Melo Euzebio, T. A.; Parra Ramirez, M. A.; Reinecke, S.; Hampel, U.

This paper presents a novel control strategy for pumps in storage tanks that accounts for fluctuations in energy prices. Storage tanks are commonly used in industrial and commercial applications to store and transport large quantities of liquids or gases. The energy consumed by pumping systems can contribute up to 20% of the total electricity usage in industrialized countries. Recent spikes in energy prices have had a detrimental impact on industries reliant on pumping systems, but the growing adoption of renewable energy sources presents new opportunities for energy demand response strategies to balance supply and demand. This study proposes a control strategy that incorporates energy price fluctuations, liquid level, input flow rate, and storm forecasting as input variables. The controller adjusts the pump flow rate every five minutes based on all four inputs. Additionally, this study highlights the environmental advantages of shifting energy usage to maximize renewable energy consumption. The simulation results on a sewer system model demonstrate a 40% reduction in wastewater volume overflow and a 15.5% reduction in energy costs compared to the results of traditional control strategies.

Keywords: Fuzzy Control; Pumps; Storage Tanks; Sewer System; Energy Price

Permalink: https://www.hzdr.de/publications/Publ-37295
Publ.-Id: 37295


Impedimetrische Nanotechnik für Bioanalytik und Diagnostik

Sandoval Bojorquez, D. I.; Janićijević, Ž.; Baraban, L.

Ultrakompakte Biosensoren in Nanogröße könnten in naher Zukunft eine ernsthafte Alternative zu modernen Systemen für die Vor-Ort-Diagnose darstellen. Impedimetrische Bionanosensoren gehören zur Gruppe der elektronischen Detektoren, die aus nanostrukturierten Elektroden bestehen, die mit einer Schicht biofunktioneller Moleküle überzogen sind, um eine hohe Spezifität für den gewünschten Analyten zu erreichen. Nach dem elektrischen Anschluss und dem Anlegen eines Wechselstrom-Eingangssignals wirkt der impedimetrische Bionanosensor wie ein durchlässiger Nanokondensator. Veränderungen in den Eigenschaften des Nanokondensators können mit der biochemischen Bindung der Moleküle und der Veränderung der elektrischen Eigenschaften der gesamten Molekülschicht in Verbindung gebracht werden. Diese Modulation der Eigenschaften des Nanokondensators kann in Echtzeit gemessen werden, indem die Änderungen der Amplitude und Phase der Ausgangswechselspannung überwacht werden.

Keywords: Impendimetrische Biosensorik; Impedanzspektroskopie (EIS); On-chip-Nanotechnologie; Nanobiosensoren; Biomarker-Analytik; Bioanalytik; Diagnostik

  • Open Access Logo Wiley Analytical Science Magazine (2023)

Permalink: https://www.hzdr.de/publications/Publ-37294
Publ.-Id: 37294


Fate of bubble clusters rising in a quiescent liquid

Ma, T.; Hessenkemper, H.; Lucas, D.; Bragg, A.

We use experiments to study the evolution of bubble clusters in a swarm of freely rising,
deformable bubbles. A new machine learning-aided algorithm allows us to identify and track
bubbles in clusters and measure the cluster lifetimes. The results indicate that contamination in
the carrier liquid can enhance the formation of bubble clusters and prolong the cluster lifetimes.
The mean bubble rise velocities conditioned on the bubble cluster size are also explored, and we
find a positive correlation between the cluster size and the rise speed of the bubbles in the cluster,
with clustered bubbles rising up to 20% faster than unclustered bubbles.

Keywords: Bubble cluster; Surfactant; Turbulence

Permalink: https://www.hzdr.de/publications/Publ-37293
Publ.-Id: 37293


Heating in multi-layer targets at ultra-high intensity laser irradiation and the impact of density oscillation

Paschke-Brühl, F.-L.; Kluge, T.; Marre, B. E.; Garten, M.; Schramm, U.; Cowan, T.; Huang, L.; Banjafar, M.; Randolph, L.; Nakatsutsumi, M.

Article about Heating in multi-layered target upon UHI laser irradiation

Keywords: Isochoric Heating; Multi layer; PIC simulation; ultra-high intenstiy laser; plasma; GISAXS

Permalink: https://www.hzdr.de/publications/Publ-37291
Publ.-Id: 37291


A note on modeling the effects of surfactants on bubble-induced turbulence

Ma, T.; Liao, Y.; Hessenkemper, H.; Lucas, D.; Bragg, A.

The recent experimental results of Ma et al. [1] reveal that with increasing concentration of surfactants, the generated bubble-induced turbulence (BIT) increases as well, although the bubbles rise slower. We show that this phenomenon has not be considered so far in the standard Reynolds-averaged Navier-Stokes (RANS) modelling for BIT, using the ansatz with source terms added to the transport equation of turbulent kinetic energy and dissipation, respectively. Some problematic issues related to the common concepts for closure of the liquid phase turbulence kinetic energy equation are also discussed. Furthermore, we demonstrated this issue by simulating the experiments using two-fluid approach.

Keywords: surfactant; bubble-induced turbulence

Permalink: https://www.hzdr.de/publications/Publ-37289
Publ.-Id: 37289


Data repository for article: Investigation of reactor pressure vessel samples of the Greifswald NPP with focus on retrospective dosimetry

Pönitz, E.; Konheiser, J.

TrepansBlock1rep.zip, TrepansBlock4.zip: Input files and calculated spectal neutron fluences.

WWERAuswertungTrepansBlock1.zip, WWERAuswertungTrepansBlock4.zip: Files/codes for calculation of reaction rates and specific activities

VKTA-Pruefberichte.zip: Measurement protocols

Figures.zip: Figures and corresponding Origin-Files for the final draft of the article

Keywords: Retrospective Dosimetry; VVER

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Permalink: https://www.hzdr.de/publications/Publ-37288
Publ.-Id: 37288


Nuklearmedizin - Basiswissen und klinische Anwendung

Dietlein, M.; Kopka, K.; Schmidt, M.

Vorwort zur 9. Auflage
Begründet von Herrn Univ.-Prof. Dr. med. Harald Schicha und Herrn Univ.-Prof. Dr. med. Dr. rer. nat. Otmar Schober ist das Lehrbuch für Nuklearmedizin in seiner 9. Auflage im Thieme Verlag durch die u.g. Herausgeber neu aufgelegt worden. Über alle Buchkapitel hinweg wurden sowohl der Text als auch das Bildmaterial erweitert und aktualisiert. Adaptiert an die klinische Weiterentwicklung des Fachgebiets Nuklearmedizin werden in der 9. Auflage die konventionelle Nuklearmedizin, die PET/CT-Diagnostik und die nuklearmedizinische Therapie in zahlreichen aktualisierten oder neu erstellten Kapiteln abgebildet. Das bewährte einführende Kapitel zur Pathophysiologie der funktionellen Tumorbildgebung blieb erhalten, in der 9. Auflage mit eigenständigen Kapiteln für die konventionelle Nuklearmedizin und für die PET/CT.
Bei der konventionellen Nuklearmedizin wurden die aktuellen Leitlinien berücksichtigt, unter anderem bei der Indikationserweiterung der Herzbildgebung
(Amyloidose, Sarkoidose, Entzündungsdiagnostik) und bei der gastrointestinalen Diagnostik. Aktuelle Entwicklungen bei der neurologischen Diagnostik wurden aufgenommen.
Jede Tumorentität, bei der die PET/CT eine klinische Bedeutung in der Patientenversorgung erlangt hat, wurde mit einem eigenen Kapitel berücksichtigt.
Zum Zeitpunkt der Erstellung der 9. Auflage hat der Gemeinsame Bundesausschuss für inzwischen 9 Fachgebiete die PET/CT in der „Ambulanten Spezialärztlichen Versorgung“ für dezidierte Indikationen zugelassen. Diese sozialmedizinischen Aspekte werden in dem Kapitel zur PET/CT bei onkologischen Fragestellungen abgehandelt.
Die Therapiekapitel wurden erweitert und aktualisiert. Für jedes etablierte nuklearmedizinische Therapieverfahren wurde ein separates Kapitel geschaffen.
Dabei hat das verlängerte Gesamtüberleben in der Zulassungsstudie für 177Lu-PSMA-617 beim metastasierten kastrationsresistenten Prostatakarzinom
(VISION-Studie) eine weitere, breite Therapieoption für die Nuklearmedizin erschlossen.
Durch diese Umstrukturierung gewinnt das Lehrbuch in seiner 9. Auflage an Aktualität und Übersichtlichkeit. Trotz zahlreicher neuer Kapitel wurde der Umfang des Lehrbuchs konstant gehalten. Dieses Konzept eines handhabbaren Lehrbuchs hat sich über mittlerweile 3 Dekaden für die diversen Zielgruppen – Ärztinnen und Ärzte mit speziellem Interesse für das Fach Nuklearmedizin, Ärztinnen und Ärzte in Weiterbildung, Ärztinnen und Ärzte anderer Fachgebiete, Medizinstudierende, MTR/RT, Naturwissenschaftlerinnen und Naturwissenschaftler – bewährt. Die Herausgeber danken dem Thieme Verlag und den Leserinnen und Lesern für das nachhaltige Interesse an dem Querschnittsfach Nuklearmedizin.
Köln/Rossendorf, 2023
Markus Dietlein
Klaus Kopka
Matthias Schmidt

Keywords: Prinzipien der Nuklearmedizin; Physikalische Grundlagen; Radiopharmazeutische Chemie; Messtechnik; Nuklearmedizinische Untersuchungen; Qualitätssicherung; Dosimetrie; Untersuchungsverfahren; Therapieverfahren

  • Book (Editorship)
    Stuttgart: Georg Thieme Verlag KG, 2023
    570 Seiten
    ISBN: 978-3-13-243926-9
    DOI: 10.1055/b000000483

Permalink: https://www.hzdr.de/publications/Publ-37286
Publ.-Id: 37286


Radiosynthesis and biological evaluation of [¹⁸F]AG-120 for PET imaging of the mutant isocitrate dehydrogenase 1 in gliomas

Lai, T. H.; Wenzel, B.; Dukic-Stefanovic, S.; Teodoro, R.; Arnaud, L.; Maisonial-Besset, A.; Weber, V.; Moldovan, R.-P.; Meister, S.; Pietzsch, J.; Kopka, K.; Juratli, T. A.; Deuther-Conrad, W.; Toussaint, M.

Gliomas are clinically challenging tumors due to their location and invasiveness nature, which often hinder complete surgical resection. The evaluation of the isocitrate dehydrogenase mutation status has become crucial for effective patient stratification. Through a transdisciplinary approach, we have developed an 18F-labeled ligand for non-invasive assessment of the IDH1R132H variant by using positron emission tomography (PET) imaging. In this study, we successfully prepared diastereomerically pure [¹⁸F]AG-120 with a copper-mediated radiofluorination approach of the stannyl precursor 6 without azeotropic drying on a TRACERlab FX2 N radiosynthesis module. In vitro internalization studies demonstrated significantly higher uptake of [¹⁸F]AG-120 in mutant IDH1R132H-U251 human high-grade glioma cells compared to wild-type IDH1-U251 cells (0.4 vs. 0.013% applied dose/μg protein at 120 min). In vivo studies conducted in mice, exhibited the excellent metabolic stability of [¹⁸F]AG-120, with parent fractions of 85% and 91% in plasma and brain at 30 min p.i., respectively. Dynamic PET studies with [¹⁸F]AG-120 in naïve mice and orthotopic glioma rat model reveal limited blood-brain barrier permeation along with a low uptake in the brain tumor. Interestingly, there was no significant difference in uptake between mutant IDH1R132H- and wild-type IDH1-tumors (tumor-to-blood ratio [40-60min]: ~1.7 vs. ~1.3). In conclusion, our preclinical evaluation demonstrated a target-specific internalization of [¹⁸F]AG-120 in vitro, a high metabolic stability in vivo in mice, and a slightly higher accumulation of activity in IDH1R132H-glioma compared to IDH1-glioma. Overall, our findings contribute to advancing the field of molecular imaging and encourage the evaluation of [¹⁸F]AG-120 to improve diagnosis and management of gliomas and other IDH1R132H-related tumors.

Keywords: IDH mutation; ivosidenib; malignant brain tumors; orthotopic glioma xenograft model; CMRF; [¹⁸F]FET

Permalink: https://www.hzdr.de/publications/Publ-37285
Publ.-Id: 37285


Plazmová závěrka pro urychlování iontů laserem (Plasma shutter for laser-driven ion acceleration)

Matys, M.; Klimo, O.; Jirka, M.; Pšikal, J.; Proška, J.; Kuchařík, M.; Nikl, J.; Kecová, M.; Korn, G.; Bulanov, S. V.

Urychlování iontů pomocí laserových impulzů se těší zvláštní pozornosti pro svoje významné aplikace, jako je hadronová terapie v onkologii a použití v materiálové a jaderné fyzice. Použitím plazmové závěrky (velmi tenké pevnolátkové fólie – plasma shutter) je možné tvarovat profil laserového impulsu, např. zmírnění předpulzu, generace strmě stoupající náběžné hrany a lokální zvýšení intenzity. V této práci jsme simulovali danou interakci vysoce-intenzivního laserového impulsu s plazmovou závěrkou a pevnolátkovým terčem pomocí 3D particle-in-cell (PIC) simulací. Aplikace plazmové závěrky měla za následek zvýšení maximální energie iontů a snížení divergence generovaného iontového svazku. Dále jsme 2D výsledky zkombinovaly hydrodynamickými simulacemi předpulzu pro použití dvojité závěrky, jejíchž prototyp byl připraven na ČVUT. Výsledky našich 3D simulací jsou také reprezentovány prostřednictvím interaktivní vizualizace ve virtuální realitě.

(The acceleration of ions by laser pulses has received particular attention for its important applications, such as hadron therapy in oncology and applications in materials and nuclear physics. By using a plasma shutter (a very thin solid-state film), it is possible to shape the profile of the laser pulse, e.g. to reduce the prepulse, generate a steeply rising leading edge and locally increase the intensity. In this work, we simulated the given interaction of a high-intensity laser pulse with a plasma shutter and a solid-state target using 3D particle-in-cell (PIC) simulations. The application of the plasma shutter resulted in an increase in the maximum ion energy and a decrease in the divergence of the generated ion beam. Furthermore, we combined the 2D results with hydrodynamic simulations of the prepulse to apply a double shutter, a prototype of which was prepared at the CTU. The results of our 3D simulations are also represented through interactive visualization in virtual reality.)

  • Poster
    21. konferencia českých a slovenských fyzikov, 04.-07.09.2023, Bratislava, Slovenská republika

Permalink: https://www.hzdr.de/publications/Publ-37284
Publ.-Id: 37284


Data publication: Suppression of matter density growth at scales exceeding the cosmic screening length

Eingorn, M.; Yilmaz, E.; Yukselci, A. E.; Zhuk, O.

The dataset consists of matter power spectra at four redshifts (z=80,50,15,0) generated by simulating Lambda-Cold Dark Matter cosmology within the cosmic screening approach as described in the associated paper.

Keywords: inhomogeneous Universe; cosmological perturbations; cosmic screening; large-scale structure

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Permalink: https://www.hzdr.de/publications/Publ-37283
Publ.-Id: 37283


Training scripts and input data sets: Transferable Interatomic Potential for Aluminum from Ambient Conditions to Warm Dense Matter

Kumar, S.; Tahmasbi, H.; Ramakrishna, K.; Lokamani, M.; Nikolov, S.; Tranchida, J.; Wood, M. A.; Cangi, A.

Here, we provide FitSNAP and DAKOTA input scripts and DFT-MD training data sets used for the generation of transferable SNAP ML-IAP for aluminum.

Keywords: Machine Learning Potential; Warm Dense Matter

Related publications

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Permalink: https://www.hzdr.de/publications/Publ-37282
Publ.-Id: 37282


Advantages and Challenges of using CFD for Pool Scrubbing Analysis

Liao, Y.

The retention of fission products in the form of aerosols and volatile species of iodine by bubbling them into liquid solution is known as pool scrubbing. It occurs frequently during accident scenarios such as SGTR (Steam Generator Tube Rupture), core meltdown and in BWR (boiling water reactor) suppression pool and FCVS (filtered containment venting system). Pool scrubbing is featured by complex hydrodynamics. The flow regime can be divided into injection, transition and bubble rise three zones. In each zone, different phenomena or mechanisms control the scrubbing of particles, e.g. globule breakup in the injection and transition zone, and swarm effect in the rise zone. Pool scrubbing codes were mostly developed in the 1980’s and 1990’s such as SUPRA, SPRAC and BUSCA, which have been widely used in the nuclear safety analysis. One major weakness of the lumped parameter codes is that they rely on various empirical correlations and assumptions, whose validity range is often limited. For example, the globule size in the jet regime and the rise velocity of large bubbles are found to be underestimated. CFD (computational fluid dynamics) has the advantage of resolving the gas-liquid interface and flow field inside the pool, capturing the coalescence and breakup of bubbles locally and physically. In the frame of IPRESCA project, several CFD studies on pool scrubbing have been published, using both VOF and two-fluid approaches. For three-dimensional large-scale pool simulations, the interface-tracking method is mainly restricted by high computational load and insufficient mesh resolution, while two-fluid method by the limitations in closure models. Reliable modelling of the processes, e.g. globule breakup in high-velocity injection zone, multiphase turbulence, interphase heat transfer, particle removal as well as bubble burst and entrainment at the free surface, remains a challenge.

  • Lecture (Conference)
    4th meeting of IPRESCA project & 2nd International Workshop on Pool Scrubbing, 05.-06.07.2023, Frankfurt, Germany
  • Lecture (others)
    Advanced nuclear energy technology and nuclear safety, 14.-17.11.2023, Xi'an, China

Permalink: https://www.hzdr.de/publications/Publ-37280
Publ.-Id: 37280


An overview of pool scrubbing related activities @HZDR

Liao, Y.

The removal of aerosols, vapor as well as soluble gases by injecting the mixture into a water pool is referred to as pool scrubbing, which is known to be an effective means for mitigating the source term during severe nuclear accidents. The pool hydrodynamics and bubble dynamics has a significant effect on the retention efficiency, which is however still far from being understood due to the complexity of the process. One-dimensional system or lumped parameter codes are routinely used for the calculation of the decontamination factor, which describes the particle removal capability of a pool scrubbing process. These codes rely on a number of empirical correlations, e.g. for the determination of bubble size and shape, which are correlated with some global and geometrical parameters such as nozzle diameter, submergence and injection velocity. Because of limited data and knowledge, the validity of these correlations is largely limited. Computational Fluid Dynamics (CFD) has the advantage of resolving local flow field and phenomena and is able to provide more insights in the bubble dynamics. In the frame of IPRESCA project, HZDR is participating in the work package 3.1 “bubble dynamics -CFD”. The main activities include three types of CFD simulations, respectively using: a) two-fluid model, where both mono-disperse and poly-disperse approaches are investigated, b) VOF interface-tracking method, and c) hybrid method, which incorporates the two-fluid and VOF models in one framework. The results shown possibilities and challenges of CFD in applying to pool scrubbing, and further efforts are needed.

  • Lecture (Conference)
    4th meeting of IPRESCA project & 2nd International Workshop on Pool Scrubbing, 05.-06.07.2023, Frankfurt, Germany

Permalink: https://www.hzdr.de/publications/Publ-37279
Publ.-Id: 37279


Lithium-induced reorientation of few-layer MoS2 films

Sojková, M.; Píš, I.; Hrdá, J.; Vojteková, T.; Pribusová Slušná, L.; Vegso, K.; Siffalovic, P.; Nadazdy, P.; Dobročka, E.; Krbal, M.; Fons, P. J.; Munnik, F.; Magnano, E.; Hulman, M.; Bondino, F.

Molybdenum disulfide (MoS2) few-layer films have gained considerable attention for their possible applications in electronics, optics, and also as a promising material for energy conversion and storage. Intercalating alkali metals, like lithium, offers the opportunity to engineer the electronic properties of MoS2. However, the influence of lithium on the growth of MoS2 layers has not been fully explored. Here, we have studied how lithium affects the structural and optical properties of the MoS2 few-layer films prepared using a new method based on one-zone sulfurization with Li2S as a source of the lithium. This method enables incorporation of Li into octahedral and tetrahedral sites of the already prepared MoS2 films or during the MoS2 formation. Our results discover an important effect of lithium promoting the epitaxial growth and horizontal alignment of the films. Moreover, we have observed a vertical-to-horizontal reorientation in vertically aligned MoS2 films upon lithiation. The measurements show long-term stability and preserved chemical composition of the horizontally aligned Li-doped MoS2.

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37278
Publ.-Id: 37278


Sim-to-Real Transfer in Deep Learning for Agitation Evaluation of Biogas Power Plants

Heller, A.; Glösekötter, P.; Buntkiel, L.; Reinecke, S.; Annas, S.

Biogas is an important driver in carbon-neutral energy sources. Many biogas digester setups, however, are not well optimized and waste energy or fail to maximize their gas output potential. To optimize these systems, a framework was developed to measure and predict digester systems’ efficiencies by closely monitoring fluid movements. This framework includes a numerical calculation of fluid behavior (Computational Fluid Dynamics (CFD)), and Deep Learning to estimate the fluid shear-rates introduced by the agitator’s action. Additionally, a novel measurement system is presented that can measure the same metrics, as simulated, in real-world environments. Lastly, an outlook is given that presents the options and extensions of the presented setup to reduce prediction error, minimize measuring efforts further, and recommend optimization approaches to the operator.

Keywords: ANN; artificial neural networks; CNN; convolutional neural networks; deep learning; CFD; computation

  • Open Access Logo Contribution to proceedings
    9th International Conference on Time Series and Forecasting, 12.-14.07.2023, Gran Canaria, Spanien
    Engineering Proceedings 2023, 39(1), 69
    DOI: 10.3390/engproc2023039069

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Permalink: https://www.hzdr.de/publications/Publ-37277
Publ.-Id: 37277


Data publication: Relaxation effects in twisted bilayer molybdenum disulfide: structure, stability, and electronic properties

Arnold, F. M.; Ghasemifard, A.; Kuc, A. B.; Kunstmann, J.; Heine, T.

Geometry optimization
Directory `calc_structure_optimization_ReaxFF`: calculation files of the structure optimization of all studied structures, done with ReaxFF.
Directory `calc_structure_optimization_DFT`: validation calculation files of the ReaxFF-optimized structures using DFT optimization.
Electronic structure calculations
Directory `calc_electronic_properties_DFT`: calculation files of electronic structure calculations on the DFT level.
Directory `calc_electronic_properties_DFTB`: calculation files of electronic structure calculations on the DFTB level
Results
Directory `structures_rigidly_twisted`: structure files in cif format of the rigidly twisted (flat) systems, labeled by their twist angle.
Directory `structures_fully_optimized`: structure files in cif format of the fully ReaxFF-optimized systems, labeled by their twist angle.
Directory `movies`: visualization of the change of the interlayer distance landscape and the strain fields with the twist angle.
Additionally, the script `plot_interlayer_distance.py` is included, which was used to create the individual frames of the movie showing the interlayer distance.

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37276
Publ.-Id: 37276


Relaxation effects in twisted bilayer molybdenum disulfide: structure, stability, and electronic properties

Arnold, F. M.; Ghasemifard, A.; Kuc, A. B.; Kunstmann, J.; Heine, T.

Manipulating the interlayer twist angle is a powerful tool to tailor the properties of layered two-dimensional crystals. The twist angle has a determinant impact on these systems’ atomistic structure and electronic properties. This includes the corrugation of individual layers, formation of stacking domains and other structural elements, and electronic structure changes due to the atomic reconstruction and superlattice effects. However, how these properties change with the twist angle, θ, is not yet well understood. Here, we monitor the change of twisted bilayer MoS2 characteristics as a function of θ. We identify distinct structural regimes, each with particular structural and electronic properties. We employ a hierarchical approach ranging from a reactive force field through the density-functional-based tight-binding approach and density-functional theory. To obtain a comprehensive overview, we analyzed a large number of twisted bilayers with twist angles in the range of θ = 0.2◦ . . . 59.6◦. Some systems include up to half a million atoms, making structure optimization and electronic property calculation challenging. For 13◦ ⪅ θ ⪅ 47◦, the structure is well-described by a moir ́e regime composed of two rigidly twisted monolayers. At small twist angles (θ ≤ 3◦ and 57◦ ≤ θ), a domain-soliton regime evolves, where the structure contains large triangular stacking domains, separated by a network of strain solitons and short-ranged high-energy nodes. The corrugation of the layers and the emerging superlattice of solitons and stacking domains affects the electronic structure. Emerging predominant characteristic features are Dirac cones at K and kagome bands. These features flatten for θ approaching 0◦ and 60◦. Our results show at which range of θ the characteristic features of the reconstruction, namely extended stacking domains, the soliton network, and superlattice, emerge and give rise to exciting electronics. We expect our findings also to be relevant for other twisted bilayer systems.

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37275
Publ.-Id: 37275


Data publication: Implementing electronic signatures of graphene and hexagonal boron nitride in twisted bilayer molybdenum disulfide

Arnold, F. M.; Ghasemifard, A.; Kuc, A. B.; Heine, T.

"ReaxFF_structure_optimization.zip": contains the inputs and outputs for all structure optimizations for ML, BL, and tBL systems using the Reax force field, performed using LAMMPS.
" bilayer_verification_ReaxFF_with_DFT.zip": contains the inputs and outputs for verifying the results of the Reax force field by running DFT geometry optimization and total energy calculations in FHI-aims for the high-symmetry bilayer stackings.
"QATK_band_structures_and_eff_mass.zip": contains the inputs and outputs of all calculations done via QuantumATK (QATK), including calculations for ML, BL, and tBL systems on DFT and DFTB level of theory.
"TB_fit.zip": contains the Python scripts and input data (DFTB band structure) used to fit the TB Hamiltonians as described in the Methods section and shown in the Supplementary Material.
"effective_masses_from_bands.zip": contains the extraction of the effective hole masses from the bands calculated at the DFTB level of theory in QATK.

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37274
Publ.-Id: 37274


Implementing electronic signatures of graphene and hexagonal boron nitride in twisted bilayer molybdenum disulfide

Arnold, F. M.; Ghasemifard, A.; Kuc, A. B.; Heine, T.

Angeli and MacDonald reported a superlattice-imposed Dirac band in twisted bilayer molybdenum disulphide (tBL MoS2) for small twist angles towards the R_h^M (parallel) stacking. Using a hierarchical set of theoretical methods, we show that the superlattices differ for twist angles with respect to metastable R_h^M (0°) and lowest-energy H_h^h (60°) configurations. When approaching R_h^M stacking, identical domains with opposite spatial orientation emerge. They form a honeycomb superlattice, yielding Dirac bands and a lateral spin texture distribution with opposite-spin-occupied K and K’ valleys. Small twist angles towards the H_h^h configuration (60°) generate H_h^h and H_h^X stacking domains of different relative energies and, hence, different spatial extensions. This imposes a symmetry break in the moiré cell, which opens a gap between the two top-valence bands, which become flat already for relatively small moiré cells. The superlattices impose electronic superstructures resembling graphene and hexagonal boron nitride into trivial semiconductor MoS2.

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37273
Publ.-Id: 37273


Edge conductivity in PtSe2 nanostructures

Kempt, R.; Kuc, A. B.; Brumme, T.; Heine, T.

PtSe2 is a promising 2D material for nanoelectromechanical sensing and photodetection in the infrared regime. One of its most compelling features is the facile synthesis at temperatures below 500 °C, which is compatible with current back-end-of-line semiconductor processing. However, this process generates polycrystalline thin films with nanoflake-like domains of 5 to 100 nm size. To investigate the lateral quantum confinement effect in this size regime, we train a deep neural network to obtain an interatomic potential at DFT accuracy and use that to model ribbons, surfaces, nanoflakes, and nanoplatelets of PtSe2 with lateral widths between 5 to 15 nm. We determine which edge terminations are the most stable and find evidence that the electrical conductivity is localized on the edges for lateral sizes below 10 nm. This suggests that the transport channels in thin films of PtSe2 might be dominated by networks of edges, instead of transport through the layers themselves.

  • Open Access Logo Small Structures (2023), 2300222
    Online First (2023) DOI: 10.1002/sstr.202300222
  • Lecture (others)
    Workshop on ‚Big data analytical methods for complex systems‘, 19.10.2023, Wrocław, Polska

Permalink: https://www.hzdr.de/publications/Publ-37272
Publ.-Id: 37272


In-situ measurements of temperature field and Marangoni convection at hydrogen bubbles using schlieren and PTV techniques

Babich, A.; Bashkatov, A.; Yang, X.; Mutschke, G.; Eckert, K.

This work adapts the schlieren technique for in-situ measurement of temperature fields around gas bubbles growing during water electrolysis. First, the optical setup and the algorithm of data processing are explained. The method is then validated by comparing measurements near a laser-heated spherical thermocouple with numerical simulations. Further validation is obtained by comparing with temperature data measured earlier by a different method near a hydrogen bubble generated at a platinum microelectrode. The schlieren technique is shown to deliver accurate temperature distributions with an uncertainty of less than 15%. The method was then used to investigate the temperature distribution near hydrogen bubbles during growth at different cathodic potentials. Additionally, particle tracking velocimetry was used to visualize the Marangoni flow pattern generated by strong Joule heating near the bubble foot. Combining the information from schlieren and PTV imaging allows to provide a more complete understanding of the fluid dynamics and heat transfer around gas bubbles growing during electrolysis.

Keywords: Schlieren method; Marangoni convection; Microelectrode; Electrolysis; Hydrogen; Bubble dynamics

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Permalink: https://www.hzdr.de/publications/Publ-37271
Publ.-Id: 37271


LEAPS Data Strategy

Götz, A.; Le Gall, E.; Konrad, U.; Kourousias, G.; Knodel, O.; Matalgah, S.; Matilla, O.; Spruce, D.; Valceril Orti, A.; Ounsy, M.; Rod, T. H.; Schluenzen, F.

The continuous evolution of photon sources and their instrumentation enables more and new scientific endeavors at ever increasing pace. This technological evolution is accompanied by an exponential growth of data volumes of increasing complexity, which must be addressed by maximizing efficiency of scientific experiments and automation of workflows covering the entire data lifecycle, aiming to reduce data volumes while producing FAIR and open data of highest reliability. This papers briefly outlines the strategy of the league of European accelerator-based photon sources user facilities to achieve these goals collaboratively in an efficient and sustainable way which will ultimately lead to an increase in the number of publications.

Keywords: Data Science; LEAPS; Photon Science

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37270
Publ.-Id: 37270


The role of interfaces and morphology on silver diffusion in hard coatings

Cavaleiro, D.; Munnik, F.; Krause, M.; Carbo, E.; Ferreira, P. J.; Cavaleiro, A.; Fernandes, F.

One of the main approaches to increase the tool lifetime during dry machining of “hard-to-machine” aerospace alloys is self-lubrication by the incorporation of noble metals in hard matrixes with good mechanical and diffusion barrier properties. In this paper, the diffusion of an Ag-rich layer sandwiched between two layers of either TiN or TiSiN is studied by transmission electron microscopy and in situ Rutherford backscattering spectrometry. The layer stacks were subjected to annealing treatments at 600 ºC and 800 ºC for 2 hours. Three processes were found to control the diffusion of silver: the morphology of the “sandwich” layers, the formation of small voids in the involved interfaces and the sublimation of Ag in the surface at temperatures near the melting point. The study revealed that the dense TiSiN matrix allowed a significantly better control of Ag diffusion than the more open TiN matrix.

Keywords: TiN and TiSiN layer stacks; Ag diffusion; Structure; Morphology

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37269
Publ.-Id: 37269


Predicting the Electronic Structure of Matter at Scale with Machine Learning

Cangi, A.; Fiedler, L.

In this talk, I will present our recent advancements in utilizing machine learning to significantly enhance the efficiency of electronic structure calculations [1]. In particular, I will focus on our efforts to accelerate Kohn-Sham density functional theory calculations at finite temperatures by incorporating deep neural networks within the Materials Learning Algorithms framework [2,3]. Our results demonstrate substantial gains in calculation speed for metals across their melting point. Furthermore, our implementation of automated machine learning has resulted in significant savings in computational resources when identifying optimal neural network architectures, thereby laying the foundation for large-scale investigations [4]. I will also showcase our most recent breakthrough, which enables neural-network-driven electronic structure calculations for systems containing over 100,000 atoms [5]. 

[1] L. Fiedler, K. Shah, M. Bussmann, A. Cangi, Phys. Rev. Materials 6, 040301, (2022).
[2] A. Cangi, J. A. Ellis, L. Fiedler, D. Kotik, N. A. Modine, V. Oles, G. A. Popoola, S. Rajamanickam, S. Schmerler, J. A. Stephens, A. P. Thompson, MALA, https://doi.org/10.5281/zenodo.5557254 (2021).
[3] J. A. Ellis, L. Fiedler, G. A. Popoola, N. A. Modine, J. A. Stephens, A. P. Thompson, A. Cangi, Phys. Rev. B 104, 035120 (2021).
[4] L. Fiedler, N. Hoffmann, P. Mohammed, G. A. Popoola, T. Yovell, V. Oles, J. A. Ellis, S. Rajamanickam, A. Cangi, Mach. Learn.: Sci. Technol. 3, 045008 (2022).
[5] L. Fiedler, N. A. Modine, S. Schmerler, D. J. Vogel, G. A. Popoola, A. P. Thompson, S. Rajamanickam, A. Cangi, arXiv:2210.11343 (2022).

Keywords: Artificial intelligence; Machine learning; Neural networks; Electronic structure; Electronic properties; Density functional theory; Materials science

  • Invited lecture (Conferences)
    Accelerating Improvements in Density Functional Theory, 21.-25.08.2023, Lausanne, Schweiz

Permalink: https://www.hzdr.de/publications/Publ-37268
Publ.-Id: 37268


Arterial spin labeling MRI

Dijsselhof, M.; Padrela, B.; Petr, J.; Mutsaerts, H. J.

ASL was invented pre-clinically in 19901. The first human applications appeared in 1996 when the post-labeling delay (PLD) was introduced to compensate for the larger distance between labeling in the neck and readout in the brain2. The initially low clinical reliability improved with the implementation of background suppression in 19993,4, the increasing availability of 3T MRI, and the invention of pseudo-continuous ASL in 20085. In 2012, the European COST-action BM1103 "ASL In Dementia” was founded and worked towards reducing the ASL differences between MRI scanners to improve between-center reproducibility. Together with other ISMRM ASL investigators, this resulted in the 2014 consensus paper that recommended single-PLD PCASL with a 3D readout, background suppression, no vascular crushing, the acquisition of a separate M0 image, and a simplified single-compartment quantification model for clinical ASL6.

  • Book chapter
    Hai-Ling Margaret Cheng, ‪Gustav J. Strijkers‬: Quantitative Perfusion MRI: Techniques, Applications and Practical Considerations (Advances in Magnetic Resonance Technology and Applications, Vol. 11), Cambridge, Massachusetts, USA: Academic Press, 2023, 978-0-323-95209-5, 77-107
    DOI: 10.1016/B978-0-323-95209-5.00007-6
    ISSN: 2666-9099

Permalink: https://www.hzdr.de/publications/Publ-37267
Publ.-Id: 37267


Mass transfer performance and hydrodynamics of a bubble column reactor at offshore floating conditions

Heydari, N.; Larachi, F.; Kipping, R.; Schubert, M.

Hydrodynamics and mass transfer characteristics are analyzed in a bubble column subjected to simulated ship motions using a hexapod robot with six-degree-of-freedom motions. Wire-mesh sensors have been used for collecting local gas holdup and flow patterns under non-reactive conditions. Additionally, the electrical conductivity of the liquid phase during CO2 uptake was extracted to determine hydroxide ion consumption rates as an indicator of mass transfer. The two-phase flow patterns in the bubble column operating under offshore conditions deviate significantly from the stationary ones due to the buoyancy-driven lateral migration of bubbles. The consumption rates of hydroxide ions during the chemical absorption of CO2 revealed that the amplitude of oscillations imposed on the bubble column is the dominant factor for the mass transfer in moving columns. Contrarily, the effect of the oscillation frequency is negligible, which is attributed to bubble coalescence and bubble flow maldistribution in the bubble column subjected to rotational oscillations. Bubble-free zones are formed in the liquid phase because of the buoyancy effects in the column tilted from the vertical axis, while the frequency of the oscillations does not add any additional effects to the bubble kinematics. The latter is attributed to the low shear rates maintained over the range of frequencies simulating marine swells.

Permalink: https://www.hzdr.de/publications/Publ-37266
Publ.-Id: 37266


BrastBook bibliography manager

Pylypovskyi, O.

This program is designed for the management of large collections of books, papers and other publications (good enough at least up to ~ 10k of records), mainly for science-oriented writing and collaborative work between small groups of researchers. Our development team was inspired by other prominent tools like JabRef or Mendeley and has been focused on a lightweight, self-sufficient tool, which can be combined with other technologies.

BraStBook uses SQLite format to store data, Qt GUI to be cross-platform and can be combined with cloud storage like DropBox/Google Drive and Git repositories for syncing between computers and accounts of different people.

Keywords: bibliography management; scientific management

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Permalink: https://www.hzdr.de/publications/Publ-37264
Publ.-Id: 37264


Recovery of Metals from Refrigerator: A Circular Economy Approach

Garcia Paz, F. A.; Parvez, A. M.

This study presents a recycling initiative conducted at STENA Recycling GmbH, focusing on the systematic recycling of 100 refrigerators. The recycling process employed a combination of manual dismantling, depollution, and mechanical techniques. Manual dismantling followed a predefined protocol to extract various materials, while the mechanical process involved shredding, zigzag separation, magnetic separation, and eddy current separation to isolate different components. The recovered materials were analyzed and categorized, providing valuable insights into the composition of refrigerator elements. Simulations were then performed to recover metals from the ferrous and non-ferrous fractions using pyrometallurgical methods. An Electric Arc Furnace (EAF) was utilized for iron recovery, while a Re-smelter process was employed for aluminum recovery, and a reducing-oxidation process was used for copper recovery. HSC Sim software and FactSage were utilized for accurate thermodynamic calculations and simulations. Furthermore, the environmental impact of the recycling process was evaluated through a Life Cycle Assessment (LCA) using Open LCA software. The LCA analysis provided insights into the environmental burdens associated with the recycling process and facilitated the identification of potential areas for improvement. The study highlights the effective utilization of resources, waste reduction, and sustainable practices in the recycling industry, considering both material recovery and environmental considerations.

  • Invited lecture (Conferences)
    CEMEREM - Summer School, 17.07.2023, Hochschule für Technik und Wirtschaft Dresden, Germany

Permalink: https://www.hzdr.de/publications/Publ-37262
Publ.-Id: 37262


X-ray imaging of two-phase flow regimes in a liquid metal swirling downward flow with side wall gas injection

Timmel, K.; Shevchenko, N.; Fujita, K.; Tsukaguchi, Y.; Eckert, S.

The formation and behavior of gas bubbles is experimentally investigated in a liquid metal downward pipe flow, a configuration that largely corresponds to the situation in a submerged entry nozzle (SEN) in the continuous casting process in steel making. The experimental mockup is operated at room temperature using the ternary alloy GaInSn as model fluid. Argon gas is injected through an orifice located in the SEN wall. The gas distribution in the pipe is visualized by means of the X-ray radiography. The set-up is completed by an electromagnetic stirrer, which is used to create a swirling flow in the tube. Depending on the volume flow rates of the gas and the liquid metal, as well as the intensity of the swirl flow generated by the stirrer, 4 flow regimes are observed: (1) the formation of an almost stationary gas pocket in the region below the injection point without any electromagnetic stirring, (2) a twisted void zone along the side wall, (3) a straight void zone in the center of the pipe, and (4) a bubble chain in the core of the pipe flow. The experiments reveal that the wetting conditions at the inner SEN wall have a decisive influence on the resulting flow regime.

Keywords: liquid metal experiment; gas injection; two-phase flow; electromagnetic stirring; continuous casting; submerged entry nozzle

Permalink: https://www.hzdr.de/publications/Publ-37261
Publ.-Id: 37261


Dataset for "Guided acoustic waves in thin epitaxial films: experiment and inverse problem solution for NiTi"

Lünser, K.; Fähler, S.

This dataset contains data about the epitaxial NiTi film that was used in the publication "Guided acoustic waves in thin epitaxial films: experiment and inverse problem solution for NiTi". It contains the SEM, AFM, FIB and R(T) data used to characterize the film.

Keywords: NiTi; epitaxial film

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Permalink: https://www.hzdr.de/publications/Publ-37259
Publ.-Id: 37259


On-chip lateral Si:Te PIN photodiodes for room-temperature detection in the telecom optical wavelength bands

Shaikh, M. S.; Wen, S.; Catuneanu, M.-T.; Wang, M.; Erbe, A.; Prucnal, S.; Rebohle, L.; Zhou, S.; Jamshidi, K.; Helm, M.; Berencen, Y.

Photonic integrated circuits require photodetectors that operate at room temperature with sensitivity at telecom wavelengths and are suitable for integration with planar complementary-metal-oxide-semiconductor (CMOS) technology. Silicon hyperdoped with deep-level impurities is a promising material for silicon infrared detectors because of its strong room-temperature photoresponse in the short-wavelength infrared region caused by the creation of an impurity band within the silicon band gap. In this work, we present the first experimental demonstration of lateral Te-hyperdoped Si PIN photodetectors operating at room temperature in the optical telecom bands. We provide a detailed description of the fabrication process, working principle, and performance of the photodiodes, including their key figure of merits. Our results are promising for the integration of active and passive photonic elements on a single Si chip, leveraging the advantages of planar CMOS technology.

Keywords: silicon; deep-level impurities; Te-hyperdoping; infrared photodetector

Related publications

  • Open Access Logo Optics Express 31(2023)16, 26451-26462
    DOI: 10.1364/OE.494463
    arXiv: https://arxiv.org/abs/2305.01374

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Permalink: https://www.hzdr.de/publications/Publ-37258
Publ.-Id: 37258


Data publication: Personnel Scheduling during the COVID-19 Pandemic: A Probabilistic Graph-Based Approach

Davoodi Monfared, M.; Batista, A.; Senapati, A.; Calabrese, J.

The data includes physical contact network of employees.

Keywords: personnel scheduling; presence strategy; testing strategy; pandemic; COVID-19

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37257
Publ.-Id: 37257


Personnel Scheduling during the COVID-19 Pandemic: A Probabilistic Graph-Based Approach

Davoodi Monfared, M.; Batista, A.; Senapati, A.; Calabrese, J.

Effective personnel scheduling is crucial for organizations to match workload demands. However, staff scheduling is sometimes affected by unexpected events, such as the COVID-19 pandemic, that disrupt regular operations. Limiting the number of on-site staff in the workplace together with regular testing is an effective strategy to minimize the spread of infectious diseases like COVID-19 because they spread mostly through close contact with people. Therefore, choosing the best scheduling and testing plan that satisfies the goals of the organization and prevents the virus’s spread is essential during disease outbreaks. In this paper, we formulate these challenges in the framework of two Mixed Integer Non-linear Programming (MINLP) models. The first model aims to derive optimal staff occupancy and testing strategies to minimize the risk of infection among employees, while the second is aimed only at optimal staff occupancy under a random testing strategy. To solve the problems expressed in the models, we propose a canonical genetic algorithm as well as two commercial solvers. Using both real and synthetic contact networks of employees, our results show that following the recommended occupancy and testing strategy reduces the risk of infection 25–60% under different scenarios. The minimum risk of infection can be achieved when the employees follow a planned testing strategy. Further, vaccination status and interaction rate of employees are important factors in developing scheduling strategies that minimize the risk of infection.

Keywords: personnel scheduling; presence strategy; testing strategy; pandemic; COVID-19

Related publications

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Permalink: https://www.hzdr.de/publications/Publ-37256
Publ.-Id: 37256


Guided acoustic waves in thin epitaxial films: experiment and inverse problem solution for NiTi

Grabec, T.; Soudná, Z.; Repček, K.; Lünser, K.; Fähler, S.; Stoklasováa, P.; Sedlák, P.; Seiner, H.

Despite the fundamental and technological importance of the elastic constants, a suitable method
for their full characterization in epitaxial films is missing. Here we show that transient grating
spectroscopy (TGS) with highly 𝑘−vector-selective generation and detection of acoustic waves
is capable of determination of all independent elastic coefficients of an epitaxial thin film
grown on a single-crystalline substrate. This experimental setup enables detection of various
types of guided acoustic waves and evaluation of the directional dependence of their speeds
of propagation. For the studied model system, which is a 3 μm thin epitaxial film of the NiTi
shape memory alloy on an MgO substrate, the TGS angular maps include Rayleigh-type surface
acoustic waves as well as Sezawa-type and Love-type modes, delivering rich information on
the elastic response of the film under different straining modes. The resulting inverse problem,
which means the calculation of the elastic constants from the TGS maps, is subsequently solved
using the Ritz-Rayleigh numerical method. Using this approach, tetragonal elastic constants of
the NiTi film and their changes with the austenite→martensite phase transition are analyzed.

Keywords: guided acoustic waves; elastic anisotropy; epitaxial thin film; shape memory alloys; transient grating spectroscop; Ritz-Rayleigh method

Permalink: https://www.hzdr.de/publications/Publ-37254
Publ.-Id: 37254


Accelerating Electronic Structure Calculations with Deep Neural Networks

Brzoza, B.; Cangi, A.

Density Functional Theory (DFT) is a widely used method for computing numerous properties in materials science and chemistry. Despite its usefulness, its inherent computational scaling with system size often limits its applicability and makes large-scale simulations infeasible. Our team develops a machine-learning approach to accelerate Kohn-Sham DFT calculations using deep neural networks within the Materials Learning Algorithms (MALA) Python framework. Our method employs bispectrum descriptors to encode roto-translationally equivariant representations of atomic neighborhoods as input to the neural networks. The networks then predict the local density of states (LDOS) from which various quantities of interest can be calculated. Our MALA models are trained on DFT data which serve as the ground-truth for the machine-learning models. Our MALA models significantly reduce the computational demands compared to conventional DFT methods. In this poster, we demonstrate the efficacy of our approach on a system of hydrogen molecules under various pressure and temperature conditions, showcasing the potential of our methods for molecular systems. Furthermore, we explore the use of SE(3)-equivariant graph neural networks (equiformer GNNs) to enhance the generalizability and extrapolation capabilities of our models while further reducing the computational cost. Our results indicate that the MALA framework provides a powerful and efficient tool for accelerating Kohn-Sham DFT calculations in molecular systems. The proposed approach has the potential to revolutionize the field of materials science by enabling researchers to perform large-scale simulations and explore complex molecular systems more efficiently. This work paves the way for future research in developing advanced machine-learning algorithms for accelerating electronic structure calculations and determining properties in materials science and chemistry both accurately and efficiently.

Keywords: Density Functional Theory; Equivariant Neural Networks; Graph Neural Networks

  • Poster
    Helmholtz AI Conference 2023, 12.-14.06.2023, Hamburg, Germany

Permalink: https://www.hzdr.de/publications/Publ-37253
Publ.-Id: 37253


Multi-physics Lagrangian MHD code based on high-order finite elements

Nikl, J.; Callow, T. J.; Löffelmann, J.; Kuchařík, M.; Cangi, A.

We present advances in the development of our multi-physics hydrodynamic code, which is designed for simulations of interaction of a laser with a solid target. Unlike the classical codes in this field, it applies the Lagrangian formulation of magnetohydrodynamics, which is ideally suited for the rapid expansion or compression of the matter during the laser-target interaction. Moreover, it is based on the modern high-order curvilinear finite elements, providing the code computational efficiency, flexibility and precision. The construction and models included in code are charted and the design of the new Arbitrary Lagrangian-Eulerian extension is presented with an outline of the possible applications.

  • Poster
    High Energy Density Science Summer School, 17.-28.07.2023, UC San Diego, California, USA

Permalink: https://www.hzdr.de/publications/Publ-37252
Publ.-Id: 37252


Data Science Education for Physics Students: Automated Object Detection for lab courses

Shah, K.

This module introduces computer vision and deep learning algorithms with applications to physics problems. It covers the basics of extracting trajectories and dynamics from videos of physical phenomena, as well as how computer vision algorithms work for detection and tracking of objects. Students will gain an understanding of how information is extracted from pixels from first principles and then learn how to apply commonly used computer vision libraries. By the end of this module, participants will have an understanding of the use of computer vision and deep learning algorithms and can apply them to analyze videos from lab experiments.

  • Open Access Logo Invited lecture (Conferences)
    Data Science Education Community of Practice Workshop, 26.-28.06.2023, College Park, MD, United States of America
  • Software in external data repository
    Publication year 2023
    Programming language: Python
    System requirements: Google Colab/Local Jupyter environment
    License: MIT
    Hosted on GitHub: Link to location

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Permalink: https://www.hzdr.de/publications/Publ-37251
Publ.-Id: 37251


Immobilization of technetium by iron corrosion phases: Lessons learnt and future perspectives

Mayordomo, N.; Rodríguez, D. M.; Brendler, V.; Roßberg, A.; Scheinost, A.; Cardaio, I.; Bureika, A.; Börner, C.; Müller, K.

Technetium-99 (⁹⁹Tc) is a long-lived fission product (2.13∙10⁵ years) of uranium-235 (²³⁵U) and plutonium-239 (²³⁹Pu) and therefore, of great concern for the long-term safe management of nuclear waste. The migration of Tc in the environment is highly influenced by the redox conditions since Tc may be present in various oxidation states. Depending on the chemical properties of environmental relevant systems Tc is expected to mainly occur as Tc(VII) and as Tc(IV) under oxidizing and reducing conditions, respectively. The anion pertechnetate (Tc(VII)O₄⁻) is known to barely interact with mineral surfaces; this, in turn, enhances its migration in groundwater and favours its entry into the biosphere. On the contrary, the formation of Tc(IV) limits the migration of Tc since it forms a low soluble solid (TcO₂) and/or species whose interaction with minerals is more favourable. In the last decades Tc migration has been focused on the reduction of Tc(VII) to Tc(IV) by various reductants, such as Fe(II), Sn(II) or S(-II) either present in solution, taking part in mineral structures, (Pearce et al., 2019) or metabolically induced by microbial cascades (Newsome et al., 2014).
We have studied the immobilization of Tc by various Fe(II)-containing phases: Fe²⁺ pre-sorbed on alumina nanoparticles (Mayordomo et al., 2020), Fe(II)-Al(III) layered double hydroxide (Mayordomo et al., 2021), and Fe(II) sulfides (Rodriguez et al., 2020; Rodríguez et al., 2021). We have combined sorption experiments, with microscopic and spectroscopic techniques (scanning electron microscopy, Raman microscopy, X-ray photoelectron spectroscopy, infrared spectroscopy, and X-ray absorption spectroscopy) to elucidate the mechanisms responsible of Tc(VII) reductive immobilization.
Those works have been focused on binary systems i.e., studies of the interaction of Tc with a given reductant. However, the environment is a complex system where different components often depend on and modify each other. Thus, Tc migration is susceptible and varies upon environmental conditions and should not be studied in an isolated manner. The young investigator group TecRad (HZDR, 2022), funded by the German Federal Ministry of Education and Research, aims at analyzing Tc chemistry from a wider perspective. Our goal is to study the biogeochemical behavior of Tc when it interacts with: i) microorganisms, ii) metabolites, iii) Fe(II) minerals, and iv) Fe(II) minerals in presence of metabolites.
An important part of this project deals with implementing new spectro-electrochemical methods to monitor in-situ the behavior of Tc in solution and at interfaces as a function of the redox potential. With these tools, we aspire at characterizing the molecular structures of Tc species under a variable range of redox conditions, to broaden the understanding of the chemical behavior of the pollutant.
We aim at generating valuable thermodynamic data (complex formation constants, solubility constants of minerals, redox potentials and Tc distribution coefficients) that will be uses to implement a geochemical modeling able to explain Tc environmental fate even under different redox conditions.
The authors acknowledge the German Federal Ministry of Education and Research (BMBF) for the financial support of NukSiFutur TecRad young investigator group (02NUK072) and the German Federal Ministry of Economic Affairs and Climate Action (BMWK, former BMWi) for the financial support of Vespa II (02E11607B).

References

HZDR 2022, accessed March 29th. https://www.hzdr.de/db/Cms?pNid=1375.

Mayordomo, N., Rodríguez, D.M., Rossberg, A., Foerstendorf, H., Heim, K., Brendler, V., Müller, K., 2021. Analysis of technetium immobilization and its molecular retention mechanisms by Fe(II)-Al(III)-Cl layered double hydroxide. Chem. Eng. J. 408, 127265. doi:10.1016/j.cej.2020.127265

Mayordomo, N., Rodríguez, D.M., Schild, D., Molodtsov, K., Johnstone, E. V., Hübner, R., Shams Aldin Azzam, S., Brendler, V., Müller, K., 2020. Technetium retention by gamma alumina nanoparticles and the effect of sorbed Fe2+. J. Hazard. Mater. 388, 122066. doi:10.1016/j.jhazmat.2020.122066

Newsome, L., Morris, K., Lloyd, J.R., 2014. The biogeochemistry and bioremediation of uranium and other priority radionuclides. Chem. Geol. 363, 164–184. doi:10.1016/j.chemgeo.2013.10.034

Pearce, C.I., Moore, R.C., Morad, J.W., Asmussen, R.M., Chatterjee, S., Lawter, A.R., Levitskaia, T.G., Neeway, J.J., Qafoku, N.P., Rigali, M.J., Saslow, S.A., Szecsody, J.E., Thallapally, P.K., Wang, G., Freedman, V.L., 2019. Technetium immobilization by materials through sorption and redox-driven processes: A literature review. Sci. Total Environ. 132849. doi:10.1016/j.scitotenv.2019.06.195

Rodriguez, D.M., Mayordomo, N., Scheinost, A.C., Brendler, V., Müller, K., Stumpf, T., 2020. New insights into 99Tc(VII) removal by pyrite : A spectroscopic approach. Env. Sci. Technol. 54, 2678–2687. doi:10.1021/acs.est.9b05341

Rodríguez, D.M., Mayordomo, N., Schild, D., Shams Aldin Azzam, S., Brendler, V., Müller, K., Stumpf, T., 2021. Reductive immobilization of 99Tc(VII) by FeS2: the effect of marcasite. Chemosphere 281, 130904. doi:10.1016/j.chemosphere.2021.130904

Keywords: Technetium; Remediation; Reduction

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  • Open Access Logo Poster
    safeND 2023: Forschungssymposium des BASE, 13.-15.09.2023, Berlin, Germany
    DOI: 10.5445/IR/1000163227

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Permalink: https://www.hzdr.de/publications/Publ-37250
Publ.-Id: 37250


Chloride green rust as scavenger of technetium: immobilization and spectroscopic studies

Mayordomo, N.; Roßberg, A.; Rodríguez, D. M.; Schild, D.; Scheinost, A.; Brendler, V.; Müller, K.

Techntium-99 (⁹⁹Tc) is one of the most concerning fission products due to its long half-life (2.13∙10⁵ years) and the high mobility of the anion pertechnetate (TcO₄⁻) [1]. Tc migration decreases significantly when Tc(VII) is reduced to Tc(IV). This scavenging step can be induced by Fe(II) minerals, which have been widely studied due to their versatility, low cost, and ubiquity [2]. In addition, Fe(II) minerals will play an important role in the near-field of the nuclear waste repository, in case that corrosion of the waste canisters will occur and radioactive material be leaked in the environment.
Green rust is formed when Fe²⁺ interacts with Fe(III) minerals [3]. Thus, its presence is expected in both the near- and far-field of a repository. It is a Fe(II)-Fe(III) hydroxide that can immobilize radionuclides by adsorption, anion exchange, and reduction mechanisms. A previous work reports the interaction of green rust with Tc, but the results are limited to very narrow experimental conditions [4]. Thus, further studies are needed to both identify the optimal Tc scavenging conditions by green rust and the mechanism responsible of Tc retention.
Our studies consisted of a combination of batch contact studies, microscopic and spectroscopic analysis. Batch contact studies were performed under a wide range of conditions, i.e. pH (3.5 - 11.0), Tc concentration (nM - mM), and ionic strength (0.0 - 0.1 M). X-ray powder diffraction, Raman microscopy, X-ray photoelectron spectroscopy (XPS), and X-ray absorption spectroscopy provided information on Tc oxidation state and speciation as well as on secondary redox products related to the Tc interaction with chloride green rust (GR(Cl)). In addition, re-oxidation experiments have been performed for one year to analyze the Tc retention reversibility.
The results show that GR(Cl) removes Tc from solution with efficiencies between 80% (Kd = 8.0∙10³ mL/g) and ≈ 100% (Kd = 9.9∙10⁵ mL/g) for pH > 6.0 (Figure 1). In contrast, Tc removal for pH < 6.0 drops with decreasing pH, and ranges from 80% to 50% (Kd = 2.0∙10³ mL/g), reaching a minimum at pH 3.5.

XPS analysis reveals the predominance of Tc(IV) at all evaluated pH values (3.5 to 11.5), supporting that Tc reductive immobilization is the main retention mechanism. Re-oxidation experiments show that Tc is slowly solubilized when time increases.
The analysis of the extended X-ray absorption fine structure indicates a change of the Tc(IV) atomic environment depending on pH and Tc loading. The most probable structural rearrangements are represented by Tc(IV) sorption on Fe(III) minerals formed as secondary phases with Tc polynuclear species contribution.

The authors acknowledge the German Federal Ministry of Education and Research (BMBF) for the financial support of the NukSiFutur TecRad young investigator group (02NUK072) [5].

References
[1] Meena, A. H. and Arai, Y (2017). Environmental geochemistry of technetium. Env. Chem. Lett. 15: 241-263.
[2] Pearce, C. I. et al. (2020). Technetium immobilization by materials through sorption and redox-driven processes: A literature review. Sci. Total Environ. 716: 132849.
[3] Usman, M. et al (2018). Magnetite and green rust: Synthesis, Properties, and Environmental Applications of Mixed-Valent Iron Minerals. Chem. Rev. 118: 3251-3304.
[4] Pepper, S. et al. (2003). Treatment of radioactive wastes: An X-ray absorption spectroscopy study of the reaction of technetium with green rust. J. Colloid Interface Sci. 268: 408-412.
[5] TecRad webpage: https://www.hzdr.de/db/Cms?pNid=1375, vis. Feb 9th 2023.

Keywords: Tc; Layered double hydroxide; Immobilization; Reduction; Molecular geometry

Related publications

  • Open Access Logo Poster
    18th International Conference on the Chemistry and Migration Behaviour of Actinides and Fission Products in the Geosphere (Migration), 24.-29.09.2023, Nantes, France
    DOI: 10.5445/IR/1000162913

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Permalink: https://www.hzdr.de/publications/Publ-37249
Publ.-Id: 37249


Gold-based Coronands as Hosts for M3+ Metal ions: Ring Size Matters

Sucena, S. F.; Demirer, T. I.; Baitullina, A.; Hagenbach, A.; Grewe, J.; Spreckelmeyer, S.; März, J.; Barkleit, A.; Maia, P. I. D. S.; Nguyen, H. H.; Abram, U.

The controlled, self-assembled synthesis of multinuclear coordination compounds can be performed via different approaches. Frequently, steric, geometric and/or electronic factors located at the ligand systems predefine the way in which metal ions can assemble them to large aggregates. For the compounds in the present paper, also the Pearson’s acidities and preferred coordination geometries of the metal ions have been used as organization principles. The ligand under study, 2,6-dipicolinoylbis(N,N-diethylthiourea), H2L1ethyl, possesses ‘soft’ sulfur and ‘hard’ nitrogen and oxygen donors. One-pot reactions of this compound with [AuCl(tht)] (tht = tetrahydrothiophene) and M3+ salts (M = Sc, Y, La, Ln, Ga, In) give products with gold-based {Au3(L1ethyl)3}3+ or {Au2(L1ethyl)2}2+ coronands, which host central M3+ ions. The formation of such units is templated by the M3+ ions and the individual size of the coronand rings is dependent on the ionic radii of the central ions in a way that small ions such as Ga3+ form a [Ga{Au2(L1ethyl)2}]+ assembly, while larger ions (starting from Sc3+/In3+) establish neutral [M{Au3(L1ethyl)3}] units with nine-coordinate central ions.

Keywords: Coronands; Gold; Lanthanides; Aroylthioureas; Self-assembly

Permalink: https://www.hzdr.de/publications/Publ-37248
Publ.-Id: 37248


Interaction of technetium with metabolites, microorganisms and at the mineral-water interface: radioecological consideration

Mayordomo, N.; Cardaio, I.; Bureika, A.; Börner, C.; Müller, K.

Technetium-99 (⁹⁹Tc) is a long-lived fission product (2.13∙10⁵ years) of uranium-235 (²³⁵U) and plutonium-239 (²³⁹Pu) and therefore, of great concern for the long-term safe management of nuclear waste. The migration of Tc in the environment is highly influenced by the redox conditions, since Tc may be present in various oxidation states. Under environmental conditions, Tc is expected to mainly occur as Tc(VII) under oxidizing conditions and as Tc(IV) under reducing conditions. The anion pertechnetate (Tc(VII)O₄⁻) is known to barely interact with mineral surfaces; this, in turn, enhances its migration in groundwater and favors its entry in the biosphere. On the contrary, the formation of Tc(IV) limits the migration of Tc since it forms a low soluble solid (TcO2) and/or species whose interaction with minerals is more favorable. In the last decades Tc migration has been focused on the reduction of Tc(VII) to Tc(IV) by various reductants, such as Fe(II), Sn(II) or S(-II) either present in solution, taking part in mineral structures, [1] or metabolically induced by microbial cascades [2].
Most of the published studies have been focused on binary systems i.e., studies of the interaction of Tc with a given reductant. However, the environment is a complex system where different components often depend on and modify each other. Thus, Tc migration is susceptible and varies upon environmental conditions and should not be studied in an isolated manner. The young investigator group TecRad [3], funded by the German Federal Ministry of Education and Research, aims at analyzing Tc chemistry from a wider perspective. Our goal is to study the biogeochemical behavior of Tc when it interacts with: i) microorganisms, ii) metabolites, iii) Fe(II) minerals, and iv) Fe(II) minerals in presence of metabolites.
An important part of this project deals with implementing new spectro-electrochemical methods to monitor in situ the behavior of Tc in solution and at interfaces as a function of the redox potential. With these tools we aspire at characterizing the molecular structures of Tc species under a variable range of redox conditions, to broaden the understanding of the chemical behavior of the pollutant.
Our goal is to generate valuable thermodynamic data (complex formation constants, solubility constants of minerals, redox potentials and Tc distribution coefficients) that we will use to implement a geochemical modeling able to explain Tc environmental fate even under different redox conditions.

The authors acknowledge the German Federal Ministry of Education and Research (BMBF) for the financial support of NukSiFutur TecRad young investigator group (02NUK072).

References
[1] Pearce, C. et al. (2020). Technetium immobilization by materials through sorption and redox-driven processes: A literature review. Sci. Total Env. 716: 132849.
[2] Newsome, L. et al. (2014). The biogeochemistry and bioremediation of uranium and other prioriy radionuclides. Chem. Geol. 363: 164-184.
[3] TecRad webpage: https://www.hzdr.de/db/Cms?pNid=1375 vis on February 9th 2023.

Keywords: Technetium; Remediation; Metabolites; Minerals; Microorganisms

  • Open Access Logo Poster
    18th International Conference on the Chemistry and Migration Behaviour of Actinides and Fission Products in the Geosphere (Migration), 24.-29.09.2023, Nantes, France

Permalink: https://www.hzdr.de/publications/Publ-37247
Publ.-Id: 37247


Hybrid treatment verification based on prompt gamma-rays and fast neutrons: Multivariate modelling for proton range determination

Schellhammer, S.; Meric, I.; Löck, S.; Kögler, T.

Robust and fast in-vivo treatment verification is expected to increase the clinical efficacy of proton therapy. The combined detection of prompt gamma-rays and neutrons has rececntly been proposed for this purpose and shown to increase the monitoring accuracy. However, the potential of this technique is not fully exploited yet since the proton range reconstruction relies only on a simple landmark of the particle production distributions. Here, we apply machine learning based feature selection and multivariate modelling to improve the range reconstruction accuracy of the system in an exemplary lung cancer case in silico. We show that the mean reconstruction error of this technique is reduced by 30 \% to 50 % to a root mean squared error (RMSE) per spot of 0.4 mm, 1.0 mm, and 1.9 mm for pencil beam scanning spot intensities of 1e8, 1e7, and 1e6 initial protons, respectively. The best model performance is reached when combining distributions features of both gamma-rays and neutrons. This confirms the advantage of hybrid gamma/neutron imaging over a single-particle approach in the presented setup and increases the potential of this system to be applied clinically for proton therapy treatment verification.

Permalink: https://www.hzdr.de/publications/Publ-37246
Publ.-Id: 37246


Polynomial-Model-Based Optimization for Blackbox Objectives

Schreiber, J.; Wicaksono, D. C.; Hecht, M.

For a wide range of applications the structure of systems like Neural Networks or complex simulations, is unknown and approximation is costly or even impossible. Black-box optimization seeks to find optimal (hyper-) parameters for these systems such that a pre-defined objective function is minimized. Polynomial-Model-Based Optimization (PMBO) is a novel blackbox optimizer that finds the minimum by fitting a polynomial surrogate to the objective function.

Motivated by Bayesian optimization the model is iteratively updated according to the acquisition function Expected Improvement, thus balancing the exploitation and exploration rate and providing an uncertainty estimate of the model. PMBO is benchmarked against other state-of-the-art algorithms for a given set of artificial, analytical functions. PMBO competes successfully with those algorithms and even outperforms all of them in some cases. As the results suggest, we believe PMBO is the pivotal choice for solving blackbox optimization tasks occurring in a wide range of disciplines.

Keywords: Black Box Optimization; Interpolation; Hyper-parameter tuning; Nonconvex optimization

Permalink: https://www.hzdr.de/publications/Publ-37244
Publ.-Id: 37244


Special Issue: Machine Learning Methods in Plasma Physics

Cangi, A.; Citrin, J.; von Toussaint, U.

In recent years, research in plasma physics has made significant progress. One area of focus is the advancement of techniques for analyzing the ever-increasing amounts of data generated from experiments and simulations. This has led to the flourishing of novel machine learning and uncertainty quantification methods. Another direction of research is to enhance artificial-intelligence and machine-learning algorithms themselves by integrating knowledge about the studied systems into the inference process. This approach leads to the development of physics-informed algorithms, which take into account constraints such as energy or momentum conservation.

As machine learning and data-driven techniques continue to gain momentum in plasma physics research, we have compiled a collection of papers from authors who are actively involved in these areas. This special issue covers a wide range of topics, including physics-informed machine learning, reduced-complexity approaches, experimental design, and real-time control applications. In the following paragraphs, we provide a summary of each paper included in this issue.

The progress in the application of data-driven algorithms is largely driven by the increasing availability of training data. Accordingly, several papers in this special issue address the challenges of improved data generation, data augmentation, and data selection. Dave et al.[1] utilize generative adversial networks to synthesize time-series such as the plasma current, which can be used to train other algorithms. In the paper of Rath et al.,[2] time-series data augmentation is explored with a focus on the robust handling of outlying data points, leading to the use of Student-t processes instead of the more familiar Gaussian processes based on experimental data.

Interpolating machine-learning algorithms, such as Gaussian processes, often suffer from a super-linear run-time dependency on the amount of data. To address this challenge, Kremers et al.[3] propose a data thinning approach based on a two-step clustering that reduces the amount of redundant data. This allows for the removal of data points that have limited impact on the quality of the resulting model, reducing both computational costs and model complexity. Gaffney et al.[4] propose a different approach for collecting simulation data using ideas from active learning[5] and experimental design approaches.[6] They suggest generating simulation data primarily in information-rich regions.

In the field of artificial-intelligence and machine-learning algorithms, one recurring topic is the replacement of expensive simulator codes that encode the underlying physics processes with suitable emulators. These are algorithms that emulate the input–output relation of the simulator with significantly reduced computational effort. Depending on the application, emulators may be realized using neural networks, polynomial chaos expansions, or reduced complexity models. Emulators are often used to perform sensitivity studies or inferences that are otherwise numerically challenging using the underlying simulator. The paper of Köberl et al.[7] demonstrates such an application, analyzing the uncertainty of a 3D magnetohydrodynamic equilibrium reconstruction using an emulator based on polynomial chaos expansions. While other machine-learning methodologies are useful, neural networks are the most common emulators due to the availability of open-source libraries and generic applicability. In Honda et al.,[8] a convolutional neural network emulates gyrokinetic simulations and shows some promising generalization capabilities in predicting the heat fluxes of ions and electrons. Similarly, in Narita et al,[9] a neural network is used to compute diffusive and non-diffusive transport parameters of tokamak fusion plasmas. Cheng et al.[10] compare different machine-learning algorithms for predicting properties of helicon plasmas and conclude that their deep neural networks outperform other approaches.

Neural networks have very fast response times, which opens up the possibility of using them for real-time control or online monitoring diagnostic settings. Tang et al.[11] describe the implementation of a recurrent neural network as a disruption predictor into a control system intended to gracefully shut down the device before a damaging disruption can occur. Similarly, Morosohk et al.[12] describe an application of neural networks, using Thomson scattering diagnostic data for real-time profile reconstruction, allowing for improved machine control based on derived physics information.

The recent trend in machine learning, which incorporates physics knowledge, is reflected in the papers of T. Nishizawa[13] and T. M. Tyranowski et al.[14] In the former paper, transport parameters are inferred based on an integrated data analysis approach, using an appropriately constrained Gaussian process. In the latter paper, a reduced complexity model for the kinetic Vlasov equation is derived, taking the underlying Hamiltonian structure of the Vlasov equation into account. This model significantly improves upon standard approaches like dynamic mode decomposition or singular value decomposition.

The intersection between plasma physics research and data science is anticipated to become increasingly interconnected in the future. As such, it is our hope that this compilation of papers will serve as a valuable source of inspiration for future endeavors in this field.

Keywords: Plasma physics; Machine learning; Neural networks

Permalink: https://www.hzdr.de/publications/Publ-37243
Publ.-Id: 37243


Analyse, Planung und Umsetzung einer verteilten Informationsarchitektur für ein New Work Konzept am HZDR (Software)

Schwabe, J.

Dieser Datensatz enthält die Software, welche im Rahmen einer Bachelorarbeit entstanden ist.

Für ein neues Bürogebäude am Helmholtz-Zentrum Dresden-Rossendorf (HZDR) sollen digitale Türschilder eingeführt werden. Dieses verteilte Informationssystem soll Informationen zu aktuellen Raumbelegungen aus bestehenden Datenbanken auslesen und von einem zentralen Server aus an die einzelnen Türschild-Controller zur entsprechenden Anzeige auf sogenannten e-Paper-Displays (EPD) senden.

Dabei gliedert sich die Software der Client-Server-Architektur in zwei Teile, den Applikationsserver zur Verwaltung mehrerer Türschilder sowie den auf jeweils einem ESP8266 realisierten Client zur Repräsentation eines einzelnen Türschildes.

Aufgabe des Servers ist die Abfrage von relevanten Informationen zu den Raumbelegungen aus entsprechenden Datenquellen, die Aufbereitung dieser zu einem Anzeigebild und die Kommunikation mit den Clients zur Übertragung der Bilder an die jeweiligen Mikrocontroller.

Analog dazu stellt der Mikrocontroller als TCP-Client die Verbindung zum Applikationsserver her, empfängt das aktuelle Anzeigebild und überträgt dieses über eine serielle Schnittstelle an das EPD. Während der Inaktivität befinden sich sowohl Mikrocontroller als auch Display in einem energiesparenden Deep Sleep-Modus.

Keywords: Data Science; Data Management; Electronic Door Sign; E-Paper; New Work; Smart Office; Python; Arduino; ESP8266

Related publications

Downloads

Permalink: https://www.hzdr.de/publications/Publ-37242
Publ.-Id: 37242


Investigations on Vibrational Interpretations of Bubbles in Metal-Making Processes

Rigas, K.; Willers, B.; Eckert, S.; Glaser, B.

Vibration measurements were carried out using highly sensitive accelerometers in an experimental ladle integrated into the LIMMCAST (Liquid Metal Model for Steel Casting) facility at HZDR. The model is operated with liquid Sn–40 wt pctBi alloy at 200°C, whose physical properties are close to those of molten steel. Three accelerometers were attached to the outer wall of the LIMMCAST vessel to record the vibrations caused by the argon bubble flow in the liquid metal at different process parameters. The results obtained at the liquid metal experiments differ from those reported for water models where the relationship between root mean square (RMS) value of the vibration amplitude and the gas flow rate follows different curve shapes. Furthermore, the results of vibration measurements in the LIMMCAST model are compared with vibration measurements in a steel plant during vacuum degassing. The comparison of the RMS data shows a fairly good agreement. This indicates that the vibrations in both the industrial process and the laboratory model are caused by the same physical mechanisms, and thus, the vibration behavior in an industrial steelmaking ladle can be reproduced quite well by suitable liquid metal models. These studies on bubble flows can help to improve the understanding of industrial stirring processes and thus contribute to a better process control.

Keywords: steel making; ladle; gas stirring; vibration measurements; liquid metal model experiment

Permalink: https://www.hzdr.de/publications/Publ-37240
Publ.-Id: 37240


Experimentelle Bestimmung der Aktivierung von deutschen Druckwasserreaktoren zur Validierung der Aktivitätsberechnungen

Barkleit, A.; Rachamin, R.; Pönitz, E.; Konheiser, J.

Experimentelle Bestimmung der Aktivierung von deutschen Druckwasserreaktoren zur Validierung der Aktivitätsberechnungen

  • Lecture (Conference)
    10. RCA-Workshop, 12.-14.06.2023, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-37239
Publ.-Id: 37239


Modelling the shredding process of multi-material structures for recycling-oriented design

Heibeck, M.; Richter, J.; Mütze, T.; Filippatos, A.

A sustainable future requires a responsible handling of our material and energy resources. However, our modern products are becoming increasingly complex with respect to the material combinations and their linkages. While we engineer multi-material structures against failure for the use phase, we also need them to be dismantled in the end-of-life phase during recycling. This describes a main functional contradiction of the structure under the scope of a circular economy and sustainability.
To achieve good material-specific recovery rates, materials locked in joints have to be liberated, which is typically achieved by breaking materials and joints in mechanical shredding processes. Unfortunately, no adequate models exist currently to describe these processes, which constitutes a missing link for a recycling-oriented design.
The presented approach models the shredding of multi-material structures with adhesion joint through numerical simulations using the finite element method (FEM). For shredding, a rotary shear is employed as usual first process stage in recycling. A rotary shear consists of two counter-rotating shafts with discs and V-shaped teeth turning at a fixed speed (circumferential velocity at teeth <0.5 m/s) and exerting tensile stresses in conjunction with bending and torsion (tearing stresses) on specimens. An A-frame dummy specimen for lightweight automotive applications was used consisting of a sheet steel top-hat profile with a glass fibre-reinforced polyamide composite layer and polyamide rib structure glued to it.
LS-DYNA software was used for explicit FE analysis as well as material models that consider the plasticity and failure of different materials and their interfaces. Furthermore, simulations were performed for different load cases, representing different orientations of the test specimen relative to the rotary shear as observed in experiments. A model evaluation workflow was developed in Python and R to quantify the shredding performance in terms of the metrics liberation degree, particle sizes and energy consumption.
Simulation results show high qualitative and quantitative agreement regarding deformation, fracture and liberation phenomena observed in previous experiments, e.g., brittle breakage of polymers into many fragments, partial to full detachment of adhesion joint, as well as high degree of plastic deformation of steel that sometimes even clamped-in polymer material thus forming new form-locking joints. One highlight is the realistic estimation of the mechanical energy consumption required for shredding. However, mass losses occur due to element deletion at failure, which are observed with increasing element size of the mesh. In addition, the model underestimates the number of generated fragments especially in the small size range (< 5 mm). Better results are expected by incorporating strain-rate dependent material behaviour in the future.
The developed simulation process could be integrated into a new design assistance tool for the conceptual design phase of multi-material structures with two main outcomes. First, to provide quantitative metrics linking the design and the failure behaviour during shredding of such structures, and consequently, to estimate the impact of design decisions on the recycling phase of a product enabling a recycling-oriented design.

Keywords: recycling; shredding; finite element simulation; multi-material design

  • Lecture (Conference)
    7th ICEAF International Conference of Engineering Against Failure, 21.-23.06.2023, Spetses, Griechenland

Permalink: https://www.hzdr.de/publications/Publ-37238
Publ.-Id: 37238


Controlled bubble formation from an orifice through harmonic gas pressure modulation

Mohseni, E.; Reinecke, S.; Hampel, U.

We used acoustic pressure waves to control the bubble formation from a submerged sub-millimeter orifice. The method enables the controlled periodic formation of bubbles with a high degree of reproducibility. Therefore, we were able to generate a continuous stream of fine bubbles as small as the orifice itself. This has a high demand in many industrial applications and fundamental research at the time. Using high-speed videometry, we studied the mechanism of the bubble formation and detachment along with the effect of various parameters on the bubble size. The analysis of forces acting on a growing bubble revealed the decisive effect of the liquid inertia on the bubble detachment. Moreover, based on the experimental results, we derived new detachment criteria for the bubble departure. These criteria can be used as the boundary condition for modeling the temporal evolution of the bubble size as well as calculating the final bubble volume using the Rayleigh-Plesset equation.

Keywords: Bubble formation; Controlled formation; Acoustic waves; Modeling; Sub-millimeter orifice

Downloads

  • Secondary publication expected from 15.08.2024

Permalink: https://www.hzdr.de/publications/Publ-37237
Publ.-Id: 37237


SurfBio - Innovation hub for surface and colloid biology science

Schymura, S.; Barros, R.; Deligiozi, I.; Furlan, C.; Lapuente De Ojeda, B.; Martel-Martin, S.; Moreno, R.; Parakhonsky, B.; Rijavec, T.; Rumbo, C.; Skirtach, A.; Suarez Diez, M.; Lapanje, A.

Centered at the Jožef Stefan Institute, Ljubljana, Slovenia, five top research & innovation partners across Europe are creating an innovation hub to study microbe-colloid–surface interactions using high-tech methodologies and equipment. The SURFBIO Innovation Hub aims to provide biotechnology researchers, academic institutions, industry and policy makers with training services and assessments to optimize novel materials for a variety of applications and will offer new, industry-oriented, research services opened to industry and institutions, covering all the needs in only one Hub, and collecting the activities together. This will lead to the founding of a SURFBIO professional society to act as a network center with the goal of fostering advanced microbial materials applications throughout Europe.
Understanding the interactions of colloids (microorganisms, nanoparticles and biomolecules) with surfaces and between themselves is a key factor that can lead to improvements of advanced materials. As such the emerging field of Colloid Biology is positioned on the intersection between material science and molecular microbiology, dealing with artificial multispecies bio-aggregates, bio- films and bio-nano-constructs of bacteria and nanoparticles, to create novel advanced materials. The colloid-biological interactions can be studied and analyzed by applying different tools and techniques. Impacts of the networking activities will be:

  • high-impact research results on surface and colloid biology
  • improved knowledge transfer
  • increased patenting
  • increased peer-reviewed publications on the topic
  • expanded range of testable samples
  • contract research for industry
  • boosted interest on surface and colloid biology
  • standardization of methodologies
  • new possibilities in analytical testing
So far, two public handbooks, two webinars and two MOOCs have been prepared and are available freely via the SURFBIO website (https://surfbio.eu/) providing information and training on the colloid biological preparation and analysis of novel advanced materials for industrial application.

Keywords: innovation hub; surface science; colloid biology

  • Poster
    NanoSAFE 2023 & Nanosafety Cluster, 05.-09.06.2023, Grenoble, Frankreich

Permalink: https://www.hzdr.de/publications/Publ-37234
Publ.-Id: 37234


Characterizing environmental behavior of nanomaterials using radiolabeling approaches

Schymura, S.; Zörner, L.; Rybkin, I.; Drev, S.; Podlipec, R.; Lapanje, A.; Mansel, A.; Strok, M.; Franke, K.

In order to characterize the potential hazards of anthropogenic nanomaterials to humanity and the environment, as well as the successful implementation of SSbD approaches, it is imperative to have access to analytic tools that provide sensitive detection at low concentrations in complex media such as surface and waste water, sewage sludge, soil, biota, etc. against same element and particle backgrounds. The radiolabeling of nanomaterials provides these features for laboratory studies. We present an overview of our radiolabelling efforts with examples of their applications.
We have developed a library of radiolabelling methods for the most common anthropogenic nanomaterials, including nanoplastics, that allow us to track nanomaterials in release, mobility and uptake studies including such complex systems as waste water treatment plants, plants, water organisms and soil. The labeling techniques are the synthesis of the nanoparticles using radioactive starting materials, the binding of the radiotracer to the nanoparticles, the activation of the nanoparticles using proton/neutron irradiation, the recoil labeling utilizing the recoil of a nuclear reaction to implant a radiotracer into the nanoparticle, and the in-diffusion of radiotracers into the nanoparticles at elevated temperatures. Using these methods we have produced [105/110mAg]Ag, [124/125/131I]CNTs, [48V]TiO2, [139/141Ce]CeO2, [7Be]MWCNT, [64Cu]SiO2, [64Cu]PS, etc. for accurate quantification in complex media at an environmentally relevant low concentrations range even with a background of the same element and without complicated sample preparations necessary.
Using these approaches, we can go beyond mere quantification and gain mechanistic insights into nanomaterial behavior in the environment. For example, we have tracked the dissolution and internalization of CeO2 NP in freshwater shrimp, the dissolution of CdSe/ZnS quantum dots in waste water treatment or the size-dependent uptake of TiO2 in plants.

Keywords: Radiolabeling; Nanoparticles; Environment

  • Lecture (Conference)
    NanoSAFE 2023 & NanoSafety Cluster, 05.-09.06.2023, Grenoble, Frankreich

Permalink: https://www.hzdr.de/publications/Publ-37233
Publ.-Id: 37233


Verification & Validation of CFD predictions regarding Pressurized Thermal Shock (PTS) situations in ROCOM installation: Comparison with IAEA Benchmark

Ayad, F.; Baghdad, M.; Bouaichaoui, Y.; Höhne, T.

The current paper documents the Computational Fluid Dynamics (CFD) code validation activity, carried out at the Nuclear Research Center of Birine relevant of Atomic Energy Commission of Algeria as part of International Atomic Energy Agency (IAEA) Coordinated Research Project (CRP): Application of Computational Fluid Dynamics Codes for Nuclear Power Plant Design to assess the current capabilities of these codes and to contribute to technological progress in their verification and validation. A set of ROCOM CFD-grade test data of Pressurized Thermal Shock test (PTS) specifications was made available in the framework of this (CRP) by Helmholtz Zentrum Dresden-Rossendorf, (HZDR) Germany, to perform detailed calculations of the proposed test. The reference point is the injection of relatively cold core cooling water (ECC), which can induce buoyant stratification. The data obtained from the PTS experiment were compared with the results of Ansys-CFX calculations in this paper. Unsteady Reynolds-Averaged Navier-Stokes (URANS) model is used to examine the buoyancy-influenced flows in the reactor pressure vessel for condition where natural circulation is a dominant factor. The Shear Stress Transport (SST k-ω) turbulence model is used to take into account the turbulence effects on the mean flow. Calculation results show a good qualitative and quantitative agreement with the experiment data.

Keywords: Verification & Validation; ROCOM; mixing; ECC; Ansys-CFX; IAEA; PTS; CRP

Downloads

  • Secondary publication expected from 25.07.2024

Permalink: https://www.hzdr.de/publications/Publ-37232
Publ.-Id: 37232


Exploring Antibacterial Activity and Bacterial-Mediated Allotropic Transition of Differentially Coated Selenium Nanoparticles

Ruiz-Fresneda, M. A.; Schaefer, S.; Hübner, R.; Fahmy, K.; Merroun, M. L.

The use of metal nanoparticles (NPs) as antimicrobial agents has become a promising alternative to the problem of antibiotic-resistant bacteria and other applications. Silver nanoparticles (AgNPs) are well-known as one of the most universal biocide compounds. However, selenium nanoparticles (SeNPs) recently gained more attention as effective antimicrobial agents. This study aims to investigate the antibacterial activity of SeNPs with different surface coatings (BSA-coated, chitosan-coated, and undefined coating) on the Gram-negative Stenotrophomonas bentonitica and the Gram-positive Lysinibacillus sphaericus in comparison to AgNPs. The tested NPs had similar properties, including shape (spheres), structure (amorphous), and size (50−90 nm), but differed in their surface charge. Chitosan SeNPs exhibited a positive surface charge, while the remaining NPs assayed had a negative surface charge. We have found that cell growth and viability of both bacteria were negatively affected in the presence of the NPs, as indicated by microcalorimetry and flow cytometry. Specifically, undefined coating SeNPs displayed the highest percentage values of dead cells for both bacteria (85−91%). An increase in reactive oxygen species (ROS) production was also detected. Chitosan-coated and undefined SeNPs caused the highest amount of ROS (299.7 and 289% over untreated controls) for S. bentonitica and L. sphaericus, respectively. Based on DNA degradation levels, undefined-SeNPs were found to be the most hazardous, causing nearly 80% DNA degradation. Finally, electron microscopy revealed the ability of the cells to transform the different SeNP types (amorphous) to crystalline SeNPs (trigonal/monoclinical Se), which could have environmentally positive implications for bioremediation purposes and provide a novel green method for the formation of crystalline SeNPs. The results obtained herein demonstrate the promising potential of SeNPs for their use in medicine as antimicrobial agents, and we propose S. bentonitica and L. sphaericus as candidates for new bioremediation strategies and NP synthesis with potential applications in many fields.

Keywords: selenium; nanoparticles; antibiotic; bioremediation; applications

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37231
Publ.-Id: 37231


RADEKOR - Speziation und Transfer von Radionukliden im Menschen unter besonderer Berücksichtigung von Dekorporationsmitteln

Barkleit, A.

Projektvorstellung

  • Lecture (Conference)
    KERNthemen2023 - Impulse. Kompetenzen. Projekte, 03.-04.05.2023, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-37230
Publ.-Id: 37230


Impact of microbes on U reduction in mine water of former U mines – a remediation perspective

Krawczyk-Bärsch, E.; Newman Portela, A.; Kassahun, A.; Merroun, M. L.; Raff, J.

Environmental pollution by heavy metals and radionuclides is one of the biggest challenges which have to be solved globally. In the former U mine of the Wismut GmbH Schlema-Alberoda (Saxony, Germany), mine water is pumped to the surface, where it is treated by a conventional water treatment plant since certain amounts of U (1 mg/L) and other water pollutants can still be found despite remediation by flooding. Microbiological studies of the mine water, using 16S rRNA gene sequencing, revealed a microbial community, which is characterized by a relative abundance of indigenous microbial groups with U(VI)-reduction ability (e.g., sulfur- and iron-oxidizing bacteria and sulfate-reducing bacteria). From previous studies it is known that microbial cycling processes have a significant impact on the complete enzymatic reduction of soluble U(VI) to U(V) and U(IV) by the addition of an electron donor in low U contaminated mine water. In our experiments, a set of anoxic microcosms with mine water were supplemented with glycerol (10mM) as electron donor. The monitoring of the redox potential, pH and the concentration of U, Fe, As and SO42- revealed a substantial decrease of the U(VI) concentration of up to 98%, as well as Fe with up to 91% and SO42- up to 88% after four months, accompanied by a significant change of the redox potential. A thermodynamic Eh-pH dominance diagram calculated using Geochemist's Workbench predicted the reduction of U(VI) and the formation of a solid U(IV)-mineral. The black precipitates, which were formed during the experiments, were analyzed spectroscopically. Extended X-ray absorption fine structure (EXAFS) indicates the formation of immobile uraninite as a U(IV) solid phase. By means of high-energy-resolution fluorescence-detected X-ray absorption near-edge structure (HERFD-XANES) it was even possible to identify U(V), a highly unstable intermediate in the reduction of U(VI) to U(IV) and poorly reported in environmental samples. In electron microscopy and energy-dispersive X-ray studies (SEM/EDXS) U(IV) nanoparticles were probably detected on the surface of calcite crystals, which have formed during the reduction experiment.

The results reveal that the indigenous microbial communities in mine waters are able to modify the speciation and redox state of the soluble U(VI) to insoluble U(V) and U(IV). The in-situ biostimulation of microorganisms could thus offer an eco-friendly water remediation strategy for the management of U contaminated mine water through bioreduction and could support chemical on-site mine water treatments.

Keywords: uranium; mine water; bacteria; spectroscopy; bioremediation

Related publications

  • Contribution to proceedings
    WISSYM 2023, 25.-28.09.2023, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-37229
Publ.-Id: 37229


Review of Experimental Database to Support Nuclear Power Plant Safety Analyses in SGTR and LOCA Domains

Hózer, Z.; Adorni, M.; Arkoma, A.; Busser, V.; Bürger, B.; Dieschbourg, K.; Girault, N.; Herranz, L. E.; Iglesias, R.; Jobst, M.; Kecek, A.; Leclere, C.; Lishchuk, R.; Massone, M.; Müllner, N.; Sholomitsky, S.; Slonszki, E.; Szabó, P.; Taurines, T.; Zimmerl, R.

In the framework of the EU R2CA project the available experimental databases were reviewed to support nuclear power plant safety analyses in SGTR and LOCA domains. The review focused on the phenomena related to fuel failure, fission products release from the fuel rods and activity transport up to the environment. Furthermore, it was shown that the phenomena were covered by different scale facilities and different experimental procedures for several reactor designs and materials. Among the tests several separate effect tests and integral tests are listed and some NPP measurements were also included. It was concluded that the reviewed database, which include more than forty experimental programmes and measurement series can be considered as a reliable basis to support the development and validation of numerical models for SGTR and LOCA safety analyses.

Keywords: Loss-of-Coolant Accident (LOCA); Steam Generator Tube Rupture (SGTR)

Permalink: https://www.hzdr.de/publications/Publ-37228
Publ.-Id: 37228


Averaging over atom snapshots in linear-response TDDFT of disordered systems: A case study of warm dense hydrogen

Moldabekov, Z.; Vorberger, J.; Lokamani, M.; Dornheim, T.

Linear-response time-dependent density functional theory (LR-TDDFT) simulations of disordered extended systems require averaging over different snapshots of ion configurations to minimize finite size effects due to the snapshot-dependence of the electronic density response function and related properties. We present a consistent scheme for the computation of the macroscopic Kohn–Sham (KS) density response function connecting an average over snapshot values of charge density perturbations to the averaged values of KS potential variations. This allows us to formulate the LR-TDDFT within the adiabatic (static) approximation for the exchange–correlation (XC) kernel for disordered systems, where the static XC kernel is computed using the direct perturbation method [Moldabekov et al., J. Chem. Theory Comput. 19, 1286 (2023)]. The presented approach allows one to compute the macroscopic dynamic density response function as well as the dielectric function with a static XC kernel generated for any available XC functional. The application of the developed workflow is demonstrated for the example of warm dense hydrogen. The presented approach is applicable for various types of extended disordered systems, such as warm dense matter, liquid metals, and dense plasmas.

Keywords: Linear-response time-dependent density functional theory; disordered systems; Kohn–Sham density response; warm dense hydrogen; dense plasmas

Permalink: https://www.hzdr.de/publications/Publ-37227
Publ.-Id: 37227


Ab-initio description of warm dense matter

Dornheim, T.

Warm dense matter (WDM)---an extreme state that is characterized by extreme densities and
temperatures---has emerged as one of the most active frontiers in plasma physics and material
science. In nature, WDM occurs in astrophysical objects such as giant planet interiors and brown
dwarfs. In addition, WDM is highly important for cutting-edge technological applications such as
inertial confinement fusion and the discovery of novel materials.
In the laboratory, WDM is studied experimentally in large facilities around the globe, and new
techniques have facilitated unprecedented insights into exciting phenomena like the formation of
nano diamonds at planetary interior conditions [1]. Yet, the interpretation of these experiments
requires a reliable diagnostics based on accurate theoretical modeling, which is a notoriously
difficult task [2].
In this talk, I give an overview of recent promising developments [3] in the field of ab initio
computer simulations of WDM, which open up new avenues for the accurate description of real
materials [4]. Moreover, I show that we can extract key parameters such as the temperature of a
given sample from X-ray Thomson scattering (XRTS) measurements [5] without any models or
approximations [6].

[1] D. Kraus et al., Nature Astronomy 1, 606-611 (2017)
[2] M. Bonitz et al., Physics of Plasmas 27, 042710 (2020)
[3] T. Dornheim et al., Physics Reports 744, 1-86 (2018)
[4] M. Böhme et al., Physical Review Letters 129, 066402 (2022)
[5] R. Redmer and S. Glenzer, Reviews of Modern Physics 81, 1625 (2009)
[6] T. Dornheim et al., Nature Communications 13, 7911 (2022)

  • Invited lecture (Conferences)
    European Physical Society (EPS) Division of Plasma Physics (DPP) Meeting, 03.-07.07.2023, Bordeaux, France

Permalink: https://www.hzdr.de/publications/Publ-37226
Publ.-Id: 37226


Biodetection platforms based on the extended gate FETs

Janićijević, Ž.

The abstract was not required for this event. In the following, a brief description of the lecture content is provided. The lecture covered the following topics: 1) Fundamental mechanisms of potentiometric biosensing based on field-effect transistors (FETs); 2) Overview of FET-sensor evolution leading to the use of extended gate (EG) FET configuration; 3) Detailed comparison between the traditional ISFET/BioFET and EG FET sensor architectures; 4) Application examples of biosensing using FET biosensors with nanoscopic sensing components (Si nanowires); 5) Cost-effective immunosensor realization using of-the-shelf electronic components with sensitivity comparable to state-of-the-art nanostructured FET biosensors; 6) Mechanism of nanoparticle-based amplification of potentiometric response in EG FET biosensors.

  • Invited lecture (Conferences)
    Hengstberger Symposium on "Bioelectronics: mimicking and interfacing biological systems", 15.-17.05.2023, Heidelberg, Germany

Permalink: https://www.hzdr.de/publications/Publ-37225
Publ.-Id: 37225


Eulerian simulations of premixed submerged multiphase turbulent jet: RANS based approach

Kamble, V. V.; Rzehak, R.; Fröhlich, J.

The recovery of mineral ores greatly depends on the hydrodynamics in a froth flotation process. Turbulent jets are created inside a froth flotation cell to enhance mixing, and thus improve recovery of mineral particles. Computational Fluid Dynamics (CFD) simulations provide a means to study such two- or three-phase turbulent jet flows by using mathematical models. The purpose of the current work is to validate the Euler-Euler CFD simulations in OpenFOAM using a set of interfacial closure models to predict the behavior of multiphase turbulent jet flows. Previously, simulations using this framework and validations were carried out for bubble columns by Rzehak and Kriebitzsch (2015) and for stirred tanks with solid-liquid flows by Shi and Rzehak (2020). The baseline closure models employed include drag, shear lift, virtual mass, wall forces, and turbulent dispersion forces for the gas-liquid as well as the solid-liquid interactions. In the present contribution, new CFD simulations using this framework are reported and validated with experimental results from Sun and Faeth (1986) for bubbly jets pointing in upward direction, and from Parthasarathy and Faeth (1987) for particulate jets pointing in downward direction. Along the axial and radial direction of the jet, a reasonable agreement is observed between the experimental and simulation results. Extending the scope of the topic, an attempt is made to simulate also three-phase premixed turbulent jets using the individually validated combination of closure models for both gas-liquid and solid-liquid jets jointly in the same simulations. Suitable data to validate the overall closure models for premixed gas-solid-liquid three-phase turbulent jet flows are not available in the literature. Thus, the simulations for three-phase turbulent jets are carried out in the same setup as used previously for the gas-liquid and the solid-liquid turbulent jets. A parametric study is carried out for the interfacial forces and an attempt to understand the interaction between the disperse and accompanying continuous phase will be presented.

Keywords: Dispersed multiphase flow; Euler-Euler two-fluid model; Closure models; Premixed submerged turbulent multiphase jets; Two-phase flows

  • Lecture (Conference)
    93rd Annual Meeting of the International Association of Applied Mathematics and Mechanics, 30.05.-02.06.2023, Dresden, Germany

Permalink: https://www.hzdr.de/publications/Publ-37223
Publ.-Id: 37223


Euler-Euler simulation of multiphase submerged jets

Kamble, V. V.; Rzehak, R.; Fröhlich, J.

The Euler-Euler two-fluid framework is applied here for submerged multiphase gas-liquid and solid-liquid turbulent jets. A set of interfacial closure models that was previously established for Computational Fluid Dynamics (CFD) simulation of different geometries such as bubble columns, pipe flows, and stirred tanks by Rzehak et al. 2017 and Shi & Rzehak 2018, 2020 is employed in the present simulations. The closure models for the momentum exchange comprise of drag-, lift-, wall-, virtual mass-, and turbulent dispersion-forces. The turbulence in the liquid phase is calculated using the 𝑘−𝜔 SST model with additional terms to consider the effects of bubble- and particle-induced turbulence. An open-source CFD tool OpenFOAM, is used to perform these simulations. Validation of the CFD simulations is performed by comparison with the experimental data of Sun & Faeth 1986 for upward pointing gas-liquid jets, and Parthasarathy & Faeth 1987 for downward pointing solid-liquid jets, respectively. The results show that the closure models are able to reasonably reproduce the measured data.

Keywords: Dispersed multiphase flow; Euler-Euler two-fluid model; Closure models; Submerged turbulent-jet

  • Lecture (Conference)
    The 11th International Conference on Multiphase Flow, 03.04.-07.07.2023, Kobe, Japan

Permalink: https://www.hzdr.de/publications/Publ-37222
Publ.-Id: 37222


Augmentation of the Standalone Multiplexed Extended-Gate Field-Effect Transistor Immunosensor Response with Gold Nanoparticle/Antibody Bioconjugates

Janićijević, Ž.; Nguyen Le, T. A.; Ahmed, A.; Zilenaite, R.; Tonmoy, T. H.; Kubeil, M.; Bachmann, M.; Baraban, L.

Electronic biosensors based on the extended-gate field-effect transistor (EGFET) concept show great promise for multiplexed biosensing in clinical screening and monitoring of complex diseases at the point of care. These biosensors offer high sensitivity, simplified integration, and easy interfacing with conventional readout electronics. However, EGFET biosensors face practical limitations that hinder their widespread use, such as the need for complex nanostructuring of extended gates (EGs) and FET transducers to achieve ultra-high sensitivity and operate at low current levels (in the ~nA range).
We present a low-cost, standalone, and multiplexed EGFET immunosensor. Our system consists of a disposable sensing chip with an EG electrode array, a multiplexing module that allows reproducible switching between up to 32 EGs, and a readout module built around a commercial FET transducer using off-the-shelf electronic components. We detect the binding of IgG antibodies by indirectly monitoring the gate surface potential, operating the FET transducer in constant charge mode. To achieve high sensitivity levels (approximately 20 mV/dec) and a low detection limit (around 10 fM), comparable to state-of-the-art nanostructured EGFET biosensors, we employ an innovative assay approach. This involves labeling the analyte antibody through bioconjugation with gold nanoparticles (AuNPs), resulting in a detection limit approximately 10^4 times lower than with the gold-standard optical method for the same antibody. Remarkably, our approach leads to a 5-fold amplification of the potentiometric response compared to direct antibody detection without labeling. To understand the origin of this amplification, we analyze the impedimetric response and find that AuNPs exhibit nanoantennae-like behavior, disrupting charge uniformity within the diffusion barrier layer and producing signal amplification. These findings demonstrate the potential for creating a new cost-effective and highly sensitive potentiometric biosensing format by utilizing customized labeling of analyte biomolecules with metallic nanoparticles.

  • Lecture (Conference)
    The 2nd International conference on Nanotechnologies and BioNanoScience (NanoBio 2023), 11.-15.09.2023, Heraklion, Greece

Permalink: https://www.hzdr.de/publications/Publ-37221
Publ.-Id: 37221


Reaktive Tracer für die Positronen-Emissions-Tomographie an porösen Materialien

Schöngart, J.; Kulenkampff, J.; Fischer, C.

Die Eignung von ¹⁸F (t½ = 110 min) als konservativer Tracer für die Positronenemissionstomographie (PET) sowie seine spezifische Verwendung als reaktiver Tracer werden im Vergleich zu dem bisher nicht untersuchten ⁷⁶Br (t½ = 16,2 h) evaluiert. Der Fokus liegt zunächst auf der Sorptionskinetik an silikatischen und karbonatischen Materialien. Zusätzlich dienen die Untersuchungen zur Einschätzung der praktisch erreichbaren Datenqualität des neuen Tracers.
Ein Phantom (Modellprobe) sowie natürliche Sandsteine wurden hinsichtlich des Transportverhaltens in konstanter Strömung mit den Radiotracern ¹⁸F und ⁷⁶Br untersucht. Unterstützend zu Positronen-Emissions-Tomogrammen mit einer Ortsauflösung von 1,15 mm und einer Zeitauflösung von 2 min wurden μ-CT-Aufnahmen mit Ortsauflösungen bis 15 μm angefertigt, um Informationen über die Porengeometrie zu erhalten.
Mit K[¹⁸F] lassen sich Sorptionseffekte mit Konzentrationen <10 pmol/mm3 (bezogen auf das Ausgangsmaterial) nachweisen. An natürlichem Sandstein konnte anhand der Tracer-Durchbruchskurven gezeigt werden, dass K[⁷⁶Br] das konservative Fließverhalten selbst bei sehr großen Ionenstärken deutlich besser abbildet als K[¹⁸F]. Mit dem reaktiven Tracer ¹⁸F konnte die Bandbreite der Oberflächenreaktivität von Karbonaten in unterschiedlichen Geomaterialien quantifiziert werden.

Keywords: PET; Positronenemissionstomographie; Reaktiver Transport; reactive transport; F-18; 18F; Br-76; 76Br; sorption; calcite; Positron Emission Tomography

  • Poster
    10. RCA Workshop, 12.-14.06.2023, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-37220
Publ.-Id: 37220


Multiplexed Extended-Gate Field-Effect Transistor-Based Immunosensor with Gold Nanoparticle-Amplified Potentiometric Response

Janićijević, Ž.; Nguyen Le, T. A.; Ahmed, A.; Žilėnaitė, R.; Tonmoy, T. H.; Kubeil, M.; Bachmann, M.; Baraban, L.

To clinically evaluate complex diseases at the point of care (POC), it is crucial to have multiplexed quantitative sensing of biomolecules. This need has led to the development of ultra-sensitive and cost-effective biosensors. Electronic biosensors based on extended gate field-effect transistor (EGFET) are promising candidates for multiplexed biosensing due to their excellent sensitivity, facile integration, and straightforward interfacing with the readout electronics. Although some high-performance biosensing applications of EGFET systems have been demonstrated [1,2], current EGFET-based biosensors still need to overcome practical issues to reach broad use in POC settings, such as readout at low current levels (~nA), limited multiplexing ability, and complex customized nanofabrication of FET transducers. We demonstrate a custom standalone multiplexed EGFET-based potentiometric biosensing platform relying on modular electronics constructed with off-the-shelf components and an innovative assay format employing bioconjugates of gold nanoparticles (AuNPs) and antibodies (Abs). Our platform comprises a disposable sensing chip containing an EG electrode array functionalized with bioreceptor molecules, a multiplexing module enabling reproducible scanning of up to 32 electrodes, and a readout module based on a commercial FET operating in constant charge mode to enable indirect monitoring of gate surface potential shifts caused by analyte binding. We observe a remarkable 5-fold amplification of the potentiometric response due to the labeling of target antibodies with AuNPs in comparison with the traditional non-labeled assay. We investigate the amplification mechanism by analyzing and modeling the impedimetric response of the system and propose that AuNPs act as localized regions of high surface charge mediating the diffusion barrier layer disruption. The AuNP-enhanced response brings the sensitivity of our platform to a level comparable with fully customized potentiometric nanobiosensors while avoiding complex nanostructuring processes and enabling accurate readout with conventional electronics. Furthermore, our EGFET-based platform exhibits ~10^4-10^6 times lower detection limits than gold-standard optical methods. Our findings indicate great promise for the development of highly sensitive and low-cost EGFET-based electronic biosensing systems suited for use at the POC.

References

[1] K. Kim et al., Nature Communications, 11 (2020) 119.
[2] H. Kim et al., ACS Nano, 15, 3 (2021) 4054–4065.

  • Lecture (Conference)
    Trends in Nanotechnology (TNT2023), 28.08.-01.09.2023, Lyon, France

Permalink: https://www.hzdr.de/publications/Publ-37219
Publ.-Id: 37219


Modular droplet-based fluidics for large volume libraries of individual multiparametric codes in lab-on-chip systems

Schütt, J.; Nhalil, H.; Faßbender, J.; Klein, L.; Grosz, A.; Makarov, D.

Droplet-based lab-on-a-chip systems offer vast possibilities in manipulation, guidance, tracking and labeling of individual droplet-based bioreactors. One of the targeted application scenarios is in drug discovery where millions of unique codes are required, which is out of reach for current technologies. Here, we propose and validate a concept for the realization of multiparametric codes, where information is stored in distinct physical and chemical parameters. Exemplarily we focus on the use of impedance and magnetic sensing by monitoring ionic concentration as well as magnetic content per droplet and droplet volume. Codes based on aqueous ferrofluid droplets were prepared using a tubing-based millifluidic setup and consist of up to 6 droplets of different combinations of volumes and magnetic concentration. We demonstrate that a droplet chain of 3 single droplets of different volume with 9 different magnetic nanoparticle concentrations accompanied with 4 different ionic concentrations per droplet offers up to 3 million unique codes. The developed fluidic platform can be readily extended to other types of sensors including optical ones to boost the coding capacity even further.

Keywords: Droplet-based fluidics; micro-magnetofluidics; planar Hall effect; contactless sensing

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37217
Publ.-Id: 37217


Multi beam computed tomography scanner design for industrial multi-phase flow investigations

Bieberle, A.; Döß, A.; Löschau, M.; Schleicher, E.; Hampel, U.

We present a multi beam gamma ray computed tomography (CT) scanner design for multi-phase flow investigations in industrial apparatuses. It mainly comprises a collimated 137Cs isotopic source and an in-house developed detector arc with overall 16 scintillation detectors offering a quantum efficiency of approximately 75% and an active area of 10×10 mm² each. The detectors are operated in pulse counting mode to enable gamma photon energy discrimination. A key element for highest flexible application of the proposed CT scanner is the elaborated detector design that is concerted with a sophisticated scanning procedure that allows for multi beam projection acquisition. Thus, scanning times can be adopted to various object sizes to save measuring times while the arrangement of source and detector arc remains identical.

Keywords: gamma ray computed tomography; detector technology

  • Contribution to proceedings
    World Congress on Industrial Process Tomography, 06.-08.09.2023, Mexico City, Mexico
  • Lecture (Conference)
    World Congress on Industrial Process Tomography, 06.-08.09.2023, Mexico City, Mexico

Permalink: https://www.hzdr.de/publications/Publ-37216
Publ.-Id: 37216


Simulation code (PIConGPU) and setup for: Reduction of the electron beam divergence of laser wakefield-accelerators by integrated plasma lenses

Pausch, R.; Chang, Y.-Y.

This repository contains the exact PIConGPU version used for all simulations in the paper "Reduction of the electron beam divergence of laser wakefield-accelerators by integrated plasma lenses" and both setups for the case with and without plasma lens.

Here, only the authors of the setup are listed. PIConGPU has many more authors that can be found under: https://github.com/ComputationalRadiationPhysics/picongpu or (latest stable release: https://doi.org/10.5281/zenodo.5795557)

Keywords: PIConGPU; LWFA; plasma lens

Downloads

Permalink: https://www.hzdr.de/publications/Publ-37215
Publ.-Id: 37215


Simulation analysis for: Reduction of the electron beam divergence of laser wakefield-accelerators by integrated plasma lenses

Pausch, R.; Chang, Y.-Y.

This is a jupyter notebook used to analyze the LWFA plasma lens simulations ran at summit ORNL.

Keywords: PIConGPU; LWFA; plasma lense

Downloads

Permalink: https://www.hzdr.de/publications/Publ-37214
Publ.-Id: 37214


Adsorption of Ferritin at Nanofaceted Al2O3 Surfaces

Pothineni, B. K.; Kollmann, S.; Li, X.; Grundmeier, G.; Erb, D.; Keller, A.

The influence of nanoscale surface topography on protein adsorption is of large importance for numerous applications in medicine and technology. Herein, the adsorption of ferritin at flat and nanofaceted Al2O3 surfaces is investigated by atomic force microscopy and X-ray photoelectron spectroscopy. The nanofaceted surfaces are generated by thermal annealing at temperature above 1000 °C, which leads to the formation of faceted saw-tooth-like surface topographies with perio-dicities of about 160 nm and amplitudes of about 15 nm. Ferritin adsorption at these nanofaceted surfaces is notably suppressed at a concentration of 10 mg/ml, which is attributed to lower ad-sorption affinities of the newly formed facets. Consequently, ferritin adsorption is restricted mostly to the grooves of the saw-tooth patterns, where the proteins can maximize their contact area with the surface. However, this effect depends on the applied protein concentration, with an inverse trend being observed at 30 mg/ml. Furthermore, different ferritin adsorption behavior is observed at topographically similar nanofacet patterns fabricated at different annealing temper-atures and attributed to different step and kink densities. These results demonstrate that while protein adsorption at solid surfaces can be notably affected by nanofacet patterns, fine-tuning protein adsorption in this way requires precise control of facet properties.

Keywords: protein adsorption; ferritin; nanopatterning; self-organization; X-ray photoelectron spectroscopy; atomic force microscopy; sapphire

Permalink: https://www.hzdr.de/publications/Publ-37213
Publ.-Id: 37213


Metallic Nanowires Self-Assembled in quasi-circular Nanomolds Templated by DNA Origami

Ruiz Arce, D. D.; Jazavandi Ghamsari, S.; Erbe, A.; Samano, E. C.

The self-assembly of conducting nanostructures is currently investigated intensively in order to evaluate the feasibility of creating novel nanoelectronic devices and circuits using such pathways. In particular, methods based on so-called DNA Origami nanostructures have shown great potential in the formation of metallic nanowires. The main challenge in this method is the reproducible generation of very well-connected metallic nanostructures which may be used as interconntects in future devices. Here we use a novel design of nanowires with a quasi-circular cross-section as opposed to rectangular or uncontrolled cross-sections in earlier studies. We find indications that the reliability of the fabrication scheme is enhanced and the overall resistance of the wires is comparable to metallic nanostructures generated by electrochemistry or top-down methods. In addition, we observe that some of the nanowires are annealed when passing a current through them, which leads to a clear enhancement for the conductance. We envision that these nanowires are providing further steps towards the succesful generation of nanoelectronics using self-assembly.

Keywords: DNA nanotechnology; nanoelectronics; self-assembly; nanomaterials

Related publications

Permalink: https://www.hzdr.de/publications/Publ-37212
Publ.-Id: 37212


CD98 heavy chain as a prognostic biomarker and target for cancer treatment

Xia, P.; Dubrovska, A.

The SLC3A2 gene encodes for a cell-surface transmembrane protein CD98hc (4F2hc). Together with the light subunits (L-type amino acid transporters) LAT1 (SLC7A5), LAT2 (SLC7A8), and xCT (SLC7A11), CD98hc constitutes heterodimeric transmembrane amino acid transporters. It interacts with other surface molecules such as extracellular matrix metalloproteinase inducer CD147 (EMMPRIN) and integrins. Thus, CD98hc plays an essential role within a protein complex critical for tumor energy metabolism, proliferation, and migration and serves as a vital regulator of the stress response and tumor growth in different types of tumors. The elevated expression levels of CD98hc have been confirmed in various tumor entities, including head and neck squamous cell carcinoma (HNSCC), glioma, colon adenocarcinoma, pancreatic ductal adenocarcinoma and others. Furthermore, a high expression of CD98hc has been linked to prognosis and response to chemo- and radiotherapy. In this mini-review, we discuss the physiological functions of CD98hc, its role in the regulation of tumor stemness, metastasis, and therapy resistance, and the clinical significance of CD98hc as a tumor marker and therapeutic target.

Keywords: CD98hc; SLC3A2; LAT1; LAT2; cancer stem cells; biomarker; therapy resistance; xCT

Permalink: https://www.hzdr.de/publications/Publ-37211
Publ.-Id: 37211


AlCl3-NaCl-ZnCl2 Secondary Electrolyte in Next-Generation ZEBRA (Na-ZnCl2) battery

Kumar, S.; Ding, W.; Hoffmann, R.; Sieuw, L.; Heinz, M. V. F.; Weber, N.; Bonk, A.

Increasing demand to store intermittent renewable electricity from, e.g., photovoltaic and wind energy has led to much research and development in large-scale energy storage, for example, ZEBRA batteries (Na-NiCl2 solid electrolyte batteries). Replacing Ni with abundant and low-cost Zn makes the ZEBRA battery more cost-effective. However, few studies were done on this next-generation ZEBRA (Na-ZnCl2) battery system, particularly on its AlCl3-NaCl-ZnCl2 secondary electrolyte. Its properties like phase diagrams and vapor pressures are vital for the cell design and optimization. In our previous work, a simulation-assisted method for molten salt electrolyte selection has shown its successful application in molten salt batteries. The same method is used here to in-depth study the AlCl3-NaCl-ZnCl2 salt electrolyte in terms of its phase diagrams and vapor pressures via FactSage and thermo-analytical techniques (Differential Scanning Calorimetry (DSC) and OptiMelt), and their effects on battery performance like operation safety and charging/discharging reaction mechanism. The DSC and OptiMelt results show that the experimental data such as melting temperatures and phase changes agree well with the simulated phase diagrams. Moreover, the FactSage simulation shows that the salt vapor pressure increases significantly with increasing temperature and molar fraction of AlCl3. The obtained phase diagrams and vapor pressures will be used in the secondary electrolyte selection, cell design and battery operation.

Permalink: https://www.hzdr.de/publications/Publ-37209
Publ.-Id: 37209


Estimation of Turbulence Parameters in Pool Scrubbing Conditions

Erol, B.; Li, S.; Liao, Y.

Abstract: Pool scrubbing is a widely used technique for retaining aerosol particles. It is characterized by high gas injection flow rates and substantial topological changes in different zones within the scrubber. The scrubbing process is generally divided into injection and swarm zones based on the evolution of the gas-liquid interface topology, and different mechanisms prevail in each zone. The disintegration of large globules in the injection zone forms a swarm of stable bubbles that significantly affect the retention efficiency since scrubbing largely depends on bubble size and velocity. However, the characteristics of the pool scrubbing process, such as high momentum, a wide range of bubble sizes, and complex interactions, make numerical simulations difficult. Turbulence is a key factor affecting bubble breakup, and estimating turbulence parameters properly is essential. In bubble columns, the effect of bubble-induced turbulence is dominant compared to turbulent pipe flows. However, the contribution of shear-induced turbulence is also significant due to circulation and strong oscillation formed in the pool by high-velocity gas injection. Modeling turbulence considering both shear and bubble-induced turbulence is still challenging in multiphase simulations. In this work, two turbulence models (mixtureKEpsilon and k-omega SST) that include the bubble-induced effects in OpenFOAM are evaluated for a pool scrubbing experiment from the literature. Using the two-equation models for turbulence is the widely accepted method in numerical simulations, making the accurate estimation of the turbulence boundary conditions critical. However, most of the correlations developed to estimate the turbulence boundary conditions are for fully developed pipe flow, making it harder to use them for bubble column simulations. Therefore, special attention is paid to characterizing turbulence intensity in a bubble column and estimating inlet boundary conditions for turbulence parameters such as turbulent kinetic energy and energy dissipation. The key parameter in estimating accurate turbulence parameters at the inlet is the turbulent viscosity. It is found that the classical definition of turbulence intensity, as the ratio between fluctuation and mean velocity, leads to an unreasonably large value for bubble column simulations because the mean velocity in the pool is extremely low, consequently, inaccurate estimation of inlet turbulence boundary conditions may result. Therefore, an approach is proposed to estimate the inlet turbulence boundary conditions that satisfy a condition revealed by the sensitivity tests in the current study. According to the results, the turbulent intensity can be estimated by constraining the turbulent viscosity value to be in the range of the molecular viscosity at the inlet if the inlet Reynolds number is in the range of laminar or transitional. Thus, too high or too low values for turbulent viscosity at the inlet may lead to numerical instabilities, considering that both the liquid and gas are quasi-laminar at the inlet.

Keywords: Pool Scrubbing; Inlet Turbulence Parameter; Turbulence Modeling; Molecular Viscosity Approach; OpenFOAM

  • Open Access Logo Poster
    19th Multiphase Flow Conference and Short Course, 19.-23.06.2023, HZDR, Germany

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Permalink: https://www.hzdr.de/publications/Publ-37208
Publ.-Id: 37208


Interaction between the transferrin protein and plutonium (and thorium), what’s new?

Zurita, C.; Tsushima, S.; Lorenzo Solari, P.; Menut, D.; Dourdain, S.; Jeanson, A.; Creff, G.; Den Auwer, C.

Transferrin (Tf) is a glycoprotein that transports iron from the serum to the various organs. Several studies have highlighted that Tf can interact with metals other than Fe(III), including actinides that are chemical and radiological toxics. We propose here to report on the behavior of Th(IV) and Pu(IV) in comparison with Fe(III) upon Tf complexation. We first considered UV-Vis and IR data of the M2Tf complex (M = Fe, Th, Pu) and combined experimental EXAFS data with MD models in order to better describe the metallic coordination site. EXAFS data of the first M-O coordination sphere are consistent with the MD model considering 1 synergistic carbonate. Further EXAFS data analysis strongly suggests that contamination by Th/Pu colloids seems to occur upon Tf complexation, but this contamination seems limited. SAXS data have also been recorded for all complexes and also after the addition of DFOB in the medium. The Rg values are very close for apoTf, ThTf and PuTf, but slightly larger than for holoTf. Data suggest that the structure of the protein is more ellipsoidal than spherical, with a flattened oblate form. From this data, the following order of conformation size might be considered : holoTf < M2Tf (M = Th, Pu) < apoTf < M2Tf-DFOB (M = Fe, Th, Pu).

Permalink: https://www.hzdr.de/publications/Publ-37207
Publ.-Id: 37207


Determination of Association Constants of Macropa-based Chelators for the Stable Complexation of Barium-131 and Lanthanum-133

Blei, M. K.; Drobot, B.; Kretzschmar, J.; Pietzsch, H.-J.; Kopka, K.; Reissig, F.; Mamat, C.

Objectives
Theranostic concepts and the usage of alpha-particle emitting radionuclides belong to the emerging fields of radiopharmaceutical sciences. Especially and due to its excellent complexation properties, the chelator macropa (mcp)[1,2] was reported to be a suitable complexing agent for 225Ac conjugates[3] and as macrocycle a highly promising starting point for the development of 223/224Ra chelators as well. To follow the theranostic approaches with these alpha emitters, due to their chemical similarities 131Ba[4] for SPECT and 133La[5] for PET are available as diagnostic radionuclide surrogates of radium and actinium, respectively. In our recent study, we aim to establish a new workflow to evaluate and predict the complex stability of new chelating systems by obtaining both protonation constants for respective ligands and association constants for their metal complexes starting with mcp.

Methods
As a prerequisite for the calculation of stability constants (log(K)), the protonation constants (pKa) of mcp were determined by pH‑dependent 1H NMR studies in the first step. Based on these obtained data, the europium-mcp-complex was examined using time-resolved, laser-induced luminescence spectroscopy (TRLFS) and the log(K) was calculated as reference stability constant. Additionally, Eu-TRLFS was used to determine the Eu-mcp species during titration and pH-dependency of the complexation. The method of isothermal titration calorimetry (ITC) was used to measure the complex stability constants of La-, Ba-mcp-complex, as well as Eu-mcp-complex to value the results in comparison with TRLFS data. The evaluation and calculation of the log(K) values were carried out by parallel factor analysis (PARAFAC).

Results
Depending on the protonation ability of the functional groups found in mcp (amines and carboxylates), pKa values were obtained as well as the log(K) values for the respective mcp-complexes with Ba, Eu and La and are shown in Table 1.

Conclusion
By combining 1H-NMR, TRLFS and ITC we demonstrated a new approach to fully characterize the ligand, determine metal complex speciation, pKa values for the mcp chelator and log(K) values of the mcp complexes and agree with previous works by potentiometric titration. Furthermore, this method can be transferred to functionalized and improved chelators and their complexes with a wide variety of metal ions of radionuclides used in nuclear medicine, especially the heavy alkaline earth metal ions Ba2+ and Ra2+. Ultimately, this allows a reliable comparison of the individual affinities of the different chelators to the metal ions and thus a predictability of the complex stabilities for future radiopharmaceuticals.

Keywords: macropa; Radium-223; Actinium-225; NMR; TRLFS; ITC

  • Poster
    25th International Symposium on Radiopharmaceutical Sciences, 22.-26.05.2023, Honolulu, Hawaii, USA

Permalink: https://www.hzdr.de/publications/Publ-37206
Publ.-Id: 37206


Rigidified 18-membered hexaaza macrocycle, H4pyta (18-py2N4Ac4), as an efficient chelator for large metal radionuclides

Faltejsek, J.; Reissig, F.; Kubíček, V.; Mamat, C.; Hermann, P.

Complexes of macrocyclic ligands are commonly utilized in many medicinal applications, such as MRI contrast agents and radiopharmaceuticals. Due to their thermodynamic stability and kinetic inertness, they overcome toxicity of free heavy metal ions and, thus, enable their use in vivo. However, there is no “general” ligand suitable for any metal ion in the periodic table and, thus, useful chelator should be specially designed for each metal ion. Among metal radionuclides, there is an increasing interest in those of large elements (i.e. large metal ions) to be used for both, radiotherapy and imaging. The 18-memberred macrocycles are suitable scaffolds for the utilizations.
This contribution deals with chemistry and radiochemistry of H4pyta (18-py2N4Ac4), a parent rigidified macrocycle suitable for large metal ions. Although the ligand was synthesized in mid-nineties, there are almost no data focused on its possible utilization in radiopharmaceutical context.[2] The ligand forms thermodynamically stable complexes with Ln(III) ions. Its ten donor atoms completely wrap the large Ln(III) ions but one pendant arm is not coordinated for small Ln(III) ions. Thus, the early Ln(III) ions form more stable complexes. The Ln(III)-H4pyta complexes are 2–3 orders of magnitude more kinetically inert than those of H4dota and, thus, they will be fully stable in vivo.
Radiolabeling of H4pyta with 133La and 177Lu is, at different pH’s and temperatures, comparable with that of H4dota. Challenging experiments showed that these radiolabeled H4pyta complexes are fully resistant to transmetallation and transchelation, and show very high stability in human blood serum stability. For larger 133La, the results are much better if compared with data obtained for H4dota and macropa in the parallel experiments. For smaller 177Lu, the results are also more promising compared to those of H4dota and its analogues.
This ligand shows that the H4pyta (18-py2N4Ac4) scaffold offers new possibilities for design of chelators for radioisotopes of large metal ions from the bottom of the Periodic Table, e.g. 225Ac, and the data are promising for future conjugations and in vivo applications.

Keywords: Alpha therapy; theranostic concept; Actinium-225; Lanthanum-133

  • Lecture (Conference)
    World Molecular Imaging Congress (WMIC), 05.-09.09.2023, Prag, Tschechische Republik

Permalink: https://www.hzdr.de/publications/Publ-37205
Publ.-Id: 37205


Bestimmung von logK-Werten macropa-basierter Chelatoren für die stabile Komplexierung von 131Ba, 223/224Ra und 133La

Blei, M. K.; Drobot, B.; Kretzschmar, J.; Pietzsch, H.-J.; Kopka, K.; Mamat, C.

225Ac-Radiotracer werden mit macropa (mcp) als Chelator bereits in präklinischen Studien für die zielgerichtete Alpha-Therapie verwendet. [1] Mit dem β+-Emitter 133La bildet 225Ac ein „Matched Pair“ gemäß des theranostischen Konzeptes. [2] Ein weiteres „Matched Pair“ bilden der γ-Strahler 131Ba mit 223/224Ra. Obwohl der [131Ba]Ba-mcp-Komplex in vivo eine zu geringe Stabilität aufweist und sich freies Ba2+ in den Knochen einlagert,[3] eignet sich der Ba-mcp-Komplex als Referenz für die Entwicklung verbesserter, mcp-basierter Chelatoren. Assoziationskonstanten, ausgedrückt als logK-Werte, sind ein Maß für die Komplexstabilität. Für deren Bestimmung wurde eigens eine neue Methode entwickelt und sowohl auf mcp als Referenz als auch auf die neuen Chelatoren angewendet.

Methodik/Methods:

Die pKs-Werte der Chelatoren wurden mittels NMR-Spektroskopie bestimmt, da diese zur Berechnung der logK-Werte essentiell sind. Mithilfe der Laser-induzierten Lumineszenzspektroskopie an Europium als Fluorophor (Eu-TRLFS) wurde dann die Bildung des Eu-mcp-Komplexes untersucht, sowie die logK-Werte der mcp-Komplexe mit Ba2+ und La3+ bestimmt. Ergänzend wurde die isotherme Titrationskalorimetrie (ITC) für die Chelatisierung von La, Eu und Ba durchgeführt. Die Berechnung der logK-Werte erfolgte durch parallele Faktoranalyse.

Ergebnisse/Results:

Die pKs-Werte von macropa wurden reproduziert und lieferten logK-Werte der Ba-, Eu- und La-mcp-Komplexe von 10.2, 14.2 bzw. 14.6.

Schlussfolgerungen/Conclusions:

Der neue methodische Ansatz, eine Kombination aus NMR, TRLFS und ITC, wurde erfolgreich etabliert und ermöglicht eine präzise Vorhersagbarkeit der Komplexstabilitäten der modifizierten mcp-Liganden für zukünftige radiopharmazeutische Anwendungen in vivo.

Keywords: Komplexstabilität; Radium-223; macropa; TRLFS; ITC; NMR

  • Lecture (Conference)
    61. DGN-Jahrestagung, 19.-22.04.2023, Leipzig, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 62(2023), 149

Permalink: https://www.hzdr.de/publications/Publ-37204
Publ.-Id: 37204


Entwicklung alternativer Verbindungen für die PSMA-Therapie mit Actinium-225

Reissig, F.; Zarschler, K.; Novy, Z.; Petrik, M.; Pietzsch, H.-J.; Kopka, K.; Mamat, C.

Ziel/Aim:

Der Einsatz von Actinium-225 mit dem DOTA-Konjugat PSMA-617 befindet sich in der klinischen Entwicklung. DOTA ist jedoch nicht ideal, da hohe Temperaturen für die Markierung benötigt werden und der Komplex in vivo nicht stabil genug ist. Ziel ist es, einen besseren, macropa-basierten Chelator zu finden und mit von PSMA-617 abgeleiteten Bindungsvektoren zu verknüpfen.

Methodik/Methods:

Es wurden 4 verschiedene Konjugate hergestellt, welche sich hinsichtlich der Anzahl der Bindungsmotive sowie ihrer Fähigkeit, an Albumin zu binden, unterscheiden. Die Stabilität der markierten Komplexe wurde über 10 Tage in Puffer und Serum untersucht. Weiterhin wurden Bindungsaffinitäten und Koloniebildungsassays an PSMA-positiven LNCaP-Zellen durchgeführt. Alle Konjugate wurden hinsichtlich ihrer Organverteilung in LNCaP-Tumor-tragenden SCID-Mäusen untersucht.

Ergebnisse/Results:

Alle 4 Konjugate wurden unter milden Bedingungen radiomarkiert und zeigen bei Zugabe von Gentisinsäure die höchste Stabilität über 10 Tagen. Die Bindungsaffinitäten der Konjugate wurden als KD-Werte bestimmt und liegen zwischen (10-40) nM. Die Untersuchungen zum Zellüberleben zeigen einen therapeutischen Vorteil der bivalenten gegenüber den monovalenten Konjugaten. Alle vier Konjugate erreichten in unterschiedlichen Zeitspannen (bis 5 d p.i.) Tumoranreicherungen von (12-85) %ID/g. Unerwünschte Anreicherungen traten v. a. bei dem dimeren, albuminbindenden Konjugat in Form von Akkumulationen (Leber, Milz, Nieren) auf.

Schlussfolgerungen/Conclusions:

Die Verwendung von macropa-basierten Konjugaten für die Therapie mit Actinium‑225 oder die zukünftige Bildgebung mit Lanthan‑133 ist vorteilhaft, da die gebildeten Komplexe stabiler sind und damit eine Anreicherung der Aktivität in off-Target-Regionen verringert werden kann. Weiterhin ergibt sich ein Vorteil im Handling, da die Reaktionen schnell und bei Raumtemperatur durchgeführt werden können, was die spätere Umsetzung in eine GMP-gerechte Herstellung erleichtert.

Keywords: zielgerichtete Alphatherapie; Lanthan-133; macropa; PSMA

  • Open Access Logo Lecture (Conference)
    61. DGN-Jahrestagung, 19.-22.04.2023, Leipzig, Deutschland
  • Abstract in refereed journal
    Nuklearmedizin 62(2023), 147

Permalink: https://www.hzdr.de/publications/Publ-37203
Publ.-Id: 37203


Radiotheranostika gegen Prostatakrebs: Actinium-225-Radiokonjugate für eine verbesserte Therapie

Mamat, C.; Reissig, F.; Novy, Z.; Petrik, M.; Pietzsch, H.-J.; Kopka, K.

Das prostataspezifische Membranantigen (PSMA) ist ein hoch attraktives biologisches Target für die molekulare Bildgebung und für die zielgerichtete Radionuklidtherapie bei kastrationsresistentem Prostatakrebs (mCRPC), da es in allen Phasen der Erkrankung bei den Tumorzellen expremiert ist. Somit bieten hoch affine, PSMA-bindende Biomoleküle eine exzellente Basis zur Entwicklung von Radiokonjugaten für die Therapie mit Alphastrahlern.
Aufgrund seiner hervorragenden kernphysikalischen Eigenschaften wird zunehmend Actinium-225 für diese Zwecke in der Nuklearmedizin verwendet. Das dreiwertige Kation Ac3+ muss dazu in einem Chelator hoch stabil komplexiert werden. Um das zu realisieren, wird der Chelator macropa verwendet, welcher eine sehr hohe In-vivo-Stabilität zeigt und Radiomarkierungen unter sehr milden Bedingungen zulässt. Dieser wird mit einer bzw. zwei PSMA-bindenden Einheiten modifiziert, um den 225Ac-Komplex zu den Tumorzellen zu bringen.
Zunächst wurden zwei Actinium-225-Radiokonjugate entwickelt und deren pharmakologische Eigenschaften, z. B. die Bindung an Tumorzellen, Anreicherung im Tumor (ca. 10%ID/g für beide Konjugate) und in anderen Organen überprüft. Hier wurde ein ähnliches Verhalten festgestellt, vergleichbar mit dem Standardkonjugat 225Ac-PSMA-617. Die beiden 225Ac-Radiokonjugate wurden weiterentwickelt und mit einem Albumin-Binder (4-Iodphenylbutyrat) versehen. Dadurch wurde eine längere Blutverweilzeit, kombiniert mit einer höheren Aufnahme in den Tumor, erreicht (bis 50%ID/g Monomer, bis 120 %ID/g Dimer), um die Effektivität der Radiotherapie zu erhöhen.

Keywords: Actinium-225; zielgerichtete Alphatherapie; Albuminbinder; PSMA; macropa

  • Lecture (Conference)
    Chemiedozententagung, 13.-15.03.2023, Dresden, Deutschland

Permalink: https://www.hzdr.de/publications/Publ-37202
Publ.-Id: 37202


Equilibrium Thermodynamics of Macropa Complexes with Selected Metal Isotopes of Radiopharmaceutical Interest

Blei, M. K.; Waurick, L.; Reissig, F.; Kopka, K.; Stumpf, T.; Drobot, B.; Kretzschmar, J.; Mamat, C.

To follow the design of in vivo stable chelating systems for radiometals, a concise and straightforward method toolbox was developed combining NMR, ITC, and Eu-TRLFS. For this purpose, the macropa chelator was chosen and Lu3+, La3+, Pb2+, Ra2+, and Ba2+ as radiopharmaceutically relevant metal ions. They differ in charge (+2, +3) and coordination properties (main group vs. lanthanides). 1H NMR was used to determine four pKa values (carboxylate functions: 2.40 and 3.13; amine functions: 6.80 and 7.73). Eu-TRLFS was used to validate the exclusive existence of the Mn+:ligand 1:1 complex in the chosen pH range. ITC measurements were accomplished to determine the resulting stability constants of the desired complexes with log K values ranging from 18.5 for the Pb-mcp complex to 7.3 for the Lu-mcp complex. DFT-calculated structures nicely mirror the complexes’ order of stabilities by bonding features. Radiolabeling with macropa using ligand concentrations from 10–3 M to 10–6 M pointed out the complex stability (133La > 131Ba > 177Lu).

Keywords: Macropa; radiolabeling; theranostic concept; protonation constant; NMR; ITC; TRLFS

Permalink: https://www.hzdr.de/publications/Publ-37201
Publ.-Id: 37201


Extension of the X2 VVER-1000 benchmark by a control rod cluster ejection exercise

Bilodid, Y.; Fischer, M.; Zilly, M.; Aures, A.; Henry, R.; Kilger, R.; Kliem, S.

This paper proposes a new benchmark for VVER-1000 control rod ejection transient. The benchmark is designed for code-to-code comparison and its purpose is testing and verifications of time-dependent solvers, core models and cross section generation methodology. Four solutions obtained using different combinations of three lattice transport, two nodal neutronics, and two thermo-hydraulic codes are analyzed, demonstrating good agreement in predicting transient reactivity and power peaks and highlighting the impact of gas gap modeling and DNBR correlation on simulation results.

Keywords: X2 VVER-1000; Control Rod Ejection; DYN3D; PARCS; ATHLET

Permalink: https://www.hzdr.de/publications/Publ-37199
Publ.-Id: 37199


Solving the puzzle of hierarchical martensitic microstructures in NiTi by (111)-oriented epitaxial films

Lünser, K.; Undisz, A.; Wagner, M. F.-X.; Nielsch, K.; Fähler, S.

The martensitic microstructure decides on the functional properties of shape memory alloys. However, for the most commonly used alloy, NiTi, it is still unclear how its microstructure is built up because the analysis is hampered by grain boundaries of polycrystalline samples. Here, we eliminate grain boundaries by using epitaxially grown films in (111)B2 orientation. By combining scale-bridging microscopy with integral inverse pole figures, we solve the puzzle of the hierarchical martensitic microstructure. We identify two martensite clusters as building blocks and three kinds of twin boundaries. Nesting them at different length scales explains why habit plane variants with 〈011〉B19' twin boundaries and {942} habit planes are dominant; but also some incompatible interfaces occur. Though the observed hierarchical microstructure agrees with the phenomenological theory of martensite, the transformation path decides which microstructure forms. The combination of local and global measurements with theory allows solving the scale bridging 3D puzzle of the martensitic microstructure in NiTi exemplarily for epitaxial films.

Keywords: NiTi; martensitic microstructure; epitaxial film

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Permalink: https://www.hzdr.de/publications/Publ-37198
Publ.-Id: 37198


Bringt uns Programmieren bei

Schmidt, P.; Erxleben, F.

Fredo Erxleben vom Helmholtz-Zentrum Dresden-Rossendorf erzählt uns, wie er und seine KollegInnen WissenschaftlerInnen, DoktorantInnen und Postdocs Programmieren beibringt. Der Bedarf an Training ist riesig. Der Bedarf an Ausbildern auch.
In dieser Folge schauen wir ein wenig hinter die Kulissen und Fredo erzählt welche Herausforderungen es bei den Trainingsprogrammen gibt.

Keywords: Podcast; RSE; Research Software Engineering; Education; HIFIS; Programming; Programmierung; Lehre; Fortbildung

Permalink: https://www.hzdr.de/publications/Publ-37197
Publ.-Id: 37197


Cosmological Perturbations Engendered by Discrete Relativistic Species

Brilenkov, M.; Yilmaz, E.; Eingorn, M.

Within the extension of the ΛCDM model, allowing for the presence of neutrinos or warm dark matter, we develop the analytical cosmological perturbation theory. It covers all spatial scales where the weak gravitational field regime represents a valid approximation. Discrete particles -- the sources of the inhomogeneous gravitational field -- may be relativistic. Similarly to the previously investigated case of nonrelativistic matter, the Yukawa interaction range is naturally incorporated into the first-order scalar metric corrections.

Keywords: inhomogeneous Universe; cosmological perturbations; cosmic screening; warm dark matter; neutrinos

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Permalink: https://www.hzdr.de/publications/Publ-37196
Publ.-Id: 37196


Fragment molecular orbital method as a tool to study actinide / lanthanide-protein interaction

Tsushima, S.

In this seminar talk, I will introduce applications of fragment molecular orbital method to study the interactions between protein and lanthanide/actinide.

  • Invited lecture (Conferences)
    Seminar talk at the Theoretical Chemistry Institute of the University of Köln, 28.06.2023, Köln, Germany

Permalink: https://www.hzdr.de/publications/Publ-37195
Publ.-Id: 37195


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