Publications Repository - Helmholtz-Zentrum Dresden-Rossendorf

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35836 Publications

Improvement of TOPFLOW void fraction data using potential field simulations of the wire-mesh sensor response

Prasser, H.-M.; Beyer, M.; Lucas, D.

At the TOPFLOW test facility of the HZDR, gas-liquid two-phase flow experiments were conducted in a vertical DN200 pipe aimed at the creation of a high-quality database. A quality check of the measurement results obtained for 48 different combinations of superficial air and water velocities (water: 0.04 -1.6 m/s, air: 0.0025 - 3.2 m/s) has shown that an overestimation of the cross-section averaged void fraction by the wire-mesh sensor is evident. This finding is supported by the analysis of drift fluxes calculated from the measured void fraction and the injected flow rates of liquid and gas, which are too low, often even negative, to be physically plausible. Another indication of the overestimation is the miss of the reproduction of the gas flow rate from a multiplication of void fraction and gas velocity profiles obtained from signals of a pair of successive sensors. Reconstructed superficial gas velocities tend to exceed significantly the values known from the injected gas flow rates in the bubbly flow region. Prasser & Häfeli (2018) showed that a linear dependency between conductance and liquid holdup at a crossing point of wires delivers too high void fraction values. The application of Maxwell’s equation for the conductivity of an emulsion was instead proposed to improve results. Furthermore, the nature of frequently observed overshoots of the conductance above the calibration values was found to correspond to a real physical phenomenon. During the previous evaluation of the TOPFLOW data, these overshoots were eliminated by setting the gas fraction to zero when they occur. The paper presents the results of a reevaluation of the TOPFLOW data using an approach based on Maxwell’s equation and a correction of the overshoots instead of truncating them. It is shown that the problem of negative drift velocities is now eliminated; the match of reconstructed and injected gas velocities considerably improved.

Keywords: Gas-liquid two-phase flow; vertical pipe; wire-mesh sensor; signal processing; measuring uncertainty

  • Contribution to proceedings
    Specialists Workshop on Advanced Instrumentation and Measurement Techniques for Experiments related to Nuclear Reactor Thermal Hydraulics and Severe Accidents, 22.-25.10.2019, Livorno, Italy
  • Lecture (Conference)
    Specialists Workshop on Advanced Instrumentation and Measurement Techniques for Experiments related to Nuclear Reactor Thermal Hydraulics and Severe Accidents, 22.-25.10.2019, Livorno, Italy

Publ.-Id: 29472

Multi-fluid models for gas-liquid flows: innovative concepts

Lucas, D.

This lecture presents innovative concepts to extent the applicability of CFD-methods in the multi-fluid framework. The GENTOP-concepts allows to consider different flow morphologies including transitions between them.

Keywords: CFD; multi-fluid; Euler-Euler; GENTOP; flow pattern transition

  • Invited lecture (Conferences)
    XIII Workshop & Summer School „Modelling of Multiphase Flows in Thermo-Chemical Systems”, 13.-15.06.2019, Wieżyca, near Gdańsk, Poland

Publ.-Id: 29470

Multi-fluid models for gas-liquid flows: consolidation of CFD modelling

Lucas, D.

This lecture presents the status and strategies for the consolidation of CFD-modelling in the multi-fluid framework. This is illustrated by the example of recent research on the further qualification of the baseline model for poly-disperse bubbly flows.

Keywords: CFD; multi-fluid; Euler-Euler; baseline model; bubbly flow

  • Invited lecture (Conferences)
    XIII Workshop & Summer School „Modelling of Multiphase Flows in Thermo-Chemical Systems”, 13.-15.06.2019, Wieżyca, near Gdańsk, Poland

Publ.-Id: 29469

Status and perspectives of CFD modelling of gas-liquid flows in the multi-fluid framework

Lucas, D.

There is an increasing request to use CFD-methods for simulations on medium and large scale industrial applications, e.g. in chemical engineering, energy techniques and nuclear safety. For most of such applications the Euler-Euler two or multi-fluid approach is the only feasible one. Gas and liquid phases are represented by interpenetrating fields and the information on the interface gets lost during the averaging process which is applied to obtain the balance equations. To close these equations the corresponding local phenomena at the gas-liquid interfaces have to be considered by closure models. As recently discussed by Lucas et al. (2016) there is not yet consensus achieved in the community regarding the most appropriate closures which limits the reliability of CFD-simulations using the Euler-Euler approach. A so-called baseline model concept was proposed in that paper. Since the closure models have to reflect the local phenomena a case by case tuning is not meaningful and instead a fixed set of closure models should be defined for certain flow conditions and applied to different cases without any modification.

Different flow morphologies as bubbly flows, droplet flows and segregated flows with large interfaces have to be distinguished. These different approaches require different closure models. In addition for poly-disperse bubbly flows it may be necessary to divide the gas phase into sub-phases reflecting bubbles of different size respectively. At HZDR a baseline model for poly-disperse bubbly flows basing on the inhomogeneous MUSIG (iMUSIG) approach (Rzehak and Krepper, 2016) and a model for segregated flows basing on the AIAD model (Porombka and Höhne, 2016) have been established. Especially the baseline model for poly-disperse flows with fixed model formulations and model parameters was validated on a large number of experiments (more than 150) for different flow geometries, flow rates and material systems. There is already an acceptable agreement for many cases, but for some also clear deviations occur. It is the scientific challenge to identify the main reasons for these deviations and figure out a better model for the corresponding phenomenon. The baseline model strategy will be illustrated by the recent developments to improve the modelling of bubbly flows and a general strategy how to develop better models will be presented.

In many flow situations interfaces may vary over a large range of scales combining dispersed and segregated morphologies. To handle such flows the innovative GENTOP concept was developed (Hänsch et al., 2012). It combines the iMUSIG and AIAD approaches and allows also simulating transitions between the different morphologies. The well validated baseline models are thus part of GENTOP. Recently the concept was applied for a simulation of a boiling pipe which includes flow pattern transitions (Höhne et al., 2017). The second part of the lecture will report about these developments which aim to extend the range of applicability of CFD simulations.

The above mentioned approaches were first implemented and tested in the commercial CFD-code ANSYS-CFX. Presently a similar framework is established for the OpenSource code OpenFOAM. A GitLab based version control system allows a high level quality assurance and has a high potential for international co-operation. Joint efforts can be done to qualify the code system.

Keywords: CFD; multi-fluid; gas-liquid; bubbly flow; segregated flow

  • Invited lecture (Conferences)
    10th International Conference on Multiphase Flow, 19.-24.05.2019, Rio de Janeiro, Brazil
  • Contribution to proceedings
    10th International Conference on Multiphase Flow, 19.-24.05.2019, Rio de Janeiro, Brazil

Publ.-Id: 29468

Heterogeneous adsorption of actinides on host rocks at the pore scale: Application of an improved surface complexation model

Yuan, T.; Bollermann, T.; Fischer, C.

In Germany, Opalinus clay strata are considered as a potential host rock for the storage of high-level nuclear waste. The adsorption efficiency of actinides in the host rock at the pore scale is essential for better understanding and prediction of actinide retention at the continuum scale, i.e., core scale and above. Surface complexation models (SCM) are a powerful tool for describing adsorption processes of actinides onto mineral surfaces. At the pore scale, the surface energy is a key constraint, which is modified by multiple parameters, e.g., crystallographic orientation, crystal defects, and nanotopography [1, 2]. Current studies on SCM [3] utilize simple retention coefficients to characterize the fluid-solid interactions without considering the effect of surface energy.

In this study, calcite and phyllosilicates are considered as two important mineral types in the Opalinus clay rock. We propose an improved SCM that implements crystal surface energy to simulate Eu (III) and U(IV) adsorption processes onto the surfaces of reference crystals. The reactions and parameters describing adsorption are modified based on the experimental results, which focus on the adsorption efficiency and its dependence on surface energy at the pore scale. The preliminary results provide the quantitative insights into the actinide retention variability in the host rock at the pore scale, which contribute to a comprehensive understanding at the core scale and above.

  • Open Access Logo Invited lecture (Conferences)
    Annual Meeting of the Nuclear Chemistry Section of GDCh 2019, 25.-27.09.2019, Dresden, Germany

Publ.-Id: 29467

Message from the Guest Editor of the 16th Multiphase Flow Conference Special Issue

Lucas, D.

Selected contributions of the 16th Multiphase Flow Conference at HZDR were published in a special issue of the Open Access Journal Experimental and Computational Multiphase Flow. In this contribution an overview on the conference and a short introduction to the single papers is given.

Keywords: multiphase flow; conference

  • Open Access Logo Abstract in refereed journal
    Experimental and Computational Multiphase Flow 1(2019), 231-232
    DOI: 10.1007/s42757-019-0037-7

Publ.-Id: 29466

Multiphase numerical modeling of a pilot-scale bubble column with a fixed poly-dispersity approach

Hosseini, A.; Mereu, R.; Canu, S.; Ziegenhein, T.; Lucas, D.; Inzoli, F.

A three-dimensional numerical study of air/water bubbly flow in a cylindrical large-scale bubble column is performed using Euler-Euler approach. The main objective is to investigate the influence of different boundary conditions such as bubble size distribution, polydispersity effects (mono and bi-dispersed approach) and mass flow rate distribution at sparger. In bi-dispersed approach the population of bubbles are divided into two groups of small and large bubbles and a mean diameter is considered for each group. The division is based on the critical bubble diameter, for which the lift coefficient changes its sign from positive to negative. For air/water system Tomiyama lift coefficient model is widely used and the critical bubble diameter is equal to 5.8 mm. A new critical bubble diameter and lift force coefficient model is introduced in this study and compared with well-known Tomiyama model. The numerical predictions are compared against the experimental data and the effect of different conditions is assessed on basis of comparison of axial gas fraction (local holdup) and global holdup. Better predictions are obtained by taking into account poly dispersity of the flow with new critical bubble diameter and new lift coefficient model. Also, it was found that mass flow-rate distribution at the sparger does not affect numerical results for global and local holdup, however a different flow pattern is observed near the sparger region.

Keywords: Computational Fluid Dynamics (CFD); bubble column; critical bubble diameter; lift force coefficient

Publ.-Id: 29465

High-speed X-ray tomography of silo discharge

Stannarius, R.; Sancho Martinez, D.; Boerzsoenyi, T.; Bieberle, M.; Barthel, F.; Hampel, U.

The outflow of granular materials from storage containers with narrow outlets is studied by means of ultrafast X-ray computed tomography (UFXCT). The used acquisition speed of this tomograph (1000 fps) is high enough to allow high-speed recording of horizontal cross sections of the container during the discharge of material. Analyzing space-time plots that were generated from the tomograms, we retrieve velocity profiles and packing structures in the container. We compare hard spherical grains with soft, low-frictional hydrogel spheres. Their flow profiles are qualitatively different. While the hard spheres form stagnant zones at the container side walls, the hydrogel spheres flow in all regions of the container. Moreover, a shell-like positional arrangement of the soft spheres induced by the container walls is revealed. The results obtained for the flow field structure confirm earlier conclusions drawn from sequences of X-ray tomograms of clogged states.

Keywords: Ultrafast X-ray CT; silo flow

Related publications

Publ.-Id: 29464

Fundamentals in GPU programming

Bieberle, A.

For the 2nd TOMOCON Summer School “Process Tomography & Data Processing”, that is conducted this time in Delft, a lecture will be given about parallel data processing programming using suitable architechtures, such as graphic processing units (GPU).

Keywords: Parallelism; GPU programming; CUDA

  • Lecture (Conference)
    2nd TOMOCON Summer School “Process Tomography & Data Processing, 01.-03.07.2019, Delft, Niederlande

Publ.-Id: 29463

Nonlinear Optical Control of Chiral Charge Pumping in a Topological Weyl Semimetal

Jadidi, M. M.; Kargarian, M.; Mittendorff, M.; Aytac, Y.; Shen, B.; König-Otto, J.; Winnerl, S.; Ni, N.; Gaeta, A. L.; Murphy, T. E.; Drew, H. D.

Solids with topologically robust electronic states exhibit unusual electronic and optical transport properties that do not exist in other materials. A particularly interesting example is chiral charge pumping, the so-called chiral anomaly, in recently discovered topological Weyl semimetals, where simultaneous application of parallel DC electric and magnetic fields creates an imbalance in the number of carriers of opposite topological charge (chirality). Here, using timeresolved terahertz measurements on the Weyl semimetal TaAs in a magnetic field, we optically interrogate the chiral anomaly by dynamically pumping the chiral charges and monitoring their subsequent relaxation. Theory based on Boltzmann transport shows that the observed effects originate from an optical nonlinearity in the chiral charge pumping process. Our measurements reveal that the chiral population relaxation time is much greater than 1 ns.
The observation of terahertz-controlled chiral carriers with long coherence times and topological protection suggests the application of Weyl semimetals for quantum optoelectronic technology.

Keywords: Wyle semimetal; TaAs; chiral charge pumpping


Publ.-Id: 29462

Direct nanoscopic observation of plasma waves in the channel of a graphene feld-effect transistor

Soltani, A.; Kuschewski, F.; Bonmann, M.; Generalov, A.; Vorobiev, A.; Ludwig, F.; Wiecha, M. M.; Cibaraite, D.; Walla, F.; Winnerl, S.; Kehr, S. C.; Eng, L. M.; Stake, J.; Roskos, H. G.

Plasma waves play an important role in many solid-state phenomena and devices. They emerge as signifcant also in electronic device structures as the operation frequencies of these devices increase. A prominent example are feld-effect transistors which are increasingly being used as rectifying detectors and mixers of electromagnetic waves at gigahertz and terahertz frequencies, where they exhibit very good sensitivity even high above the cut-off frequencies which limit their application in amplifers and switches. Transport theory predicts that coupling of radiation at THz frequencies into the channel of a feld-effect transistor leads to the development of a gated plasma wave collectively involving the charge carriers of both the two-dimensional electron gas and of the gate electrode. Because of the small spatial separation of the channel from the gate, such a wave propagates with a speed much lower than the vacuum speed of light. In this paper, we present the first direct visualization of such waves. Employing graphene FETs with a buried gate electrode, we utilize near-field THz nanoscopy at room temperature to probe the electric field amplitude of the propagating wave directly on the exposed graphene sheet. Mapping of the feld distribution allows us to determine the decay length and the gate-voltage-dependent propagation speed of the plasma waves which is found to lie in the range of 3.5-7 x 10^6 m/s, in good agreement with theory.

Keywords: graphene field-effect transistor; plasma waves; near-field microscopy

Publ.-Id: 29461

Suppressed Auger scattering and tunable light emission of Landau-quantized massless Kane electrons

But, D. B.; Mittendorff, M.; Consejo, C.; Teppe, F.; Mikhailov, N. N.; Dvoretskii, S. A.; Faugeras, C.; Winnerl, S.; Helm, M.; Knap, W.; Potemski, M.; Orlita, M.

The Landau level laser has been proposed a long time ago as a unique source of monochromatic radiation, widely tunable in the THz and infrared spectral ranges using an externally applied magnetic field. In spite of decades of efforts, this appealing concept never resulted in the design of a reliable device. This is due to effcient Auger scattering of Landau-quantized electrons, which is an intrinsic non-radiative recombination channel that eventually gains over cyclotron emission in all materials studied so far: in conventional semiconductors with parabolic bands, but also in graphene with massless electrons. The Auger processes are favored in these systems by Landau levels (or their subsets) equally spaced in energy. Here we show that this scheme does not apply to massless Kane electrons in gapless HgCdTe alloy, in which undesirable Auger scattering is strongly suppressed and the sizeable cyclotron emission observed, for the first time in the case of massless particles. The gapless HgCdTe thus appears as a material of choice for future technology of Landau level lasers.

Keywords: Kane electrons; Landau quantization; Auger scattering; cyclotron emission


Publ.-Id: 29460

Holistic Data Management as a Key Towards Reproducible Science in a Diverse and Dynamic Ecosystem

Juckeland, G.

Eingeladener Vortrag an der RWTH Aachen

  • Open Access Logo Lecture (others)
    IT Seminar der RWTH Aachen, 12.07.2019, Aachen, Deutschland

Publ.-Id: 29459

High-gain quantum free-electron laser: Emergence and exponential gain

Kling, P.; Giese, E.; Carmesin, C. M.; Sauerbrey, R.; Schleich, W. P.

We derive an effective Dicke model in momentum space to describe collective effects in the quantum regime of a free-electron laser (FEL). The resulting exponential gain from a single passage of electrons allows the operation of a Quantum FEL in the high-gain mode and avoids the experimental challenges of an x-ray FEL oscillator. Moreover, we study the intensity fluctuations of the emitted radiation, which turn out to be super-Poissonian.

Keywords: Quantum Free Electron Laser; Quantum FEL; Free Electron Laser; QFEL; FEL; Dicke model

Publ.-Id: 29457

Experimental and numerical studies on high-pressure Steam Condensation in a horizontal condenser tube

Bieberle, A.; Moonesi Shabestary, A.; Boden, S.; Beyer, M.; Unger, S.; Lucas, D.; Hampel, U.

We introduce results of an experimental and numerical study on condensation steam heat transfer in a near horizontal tube at pressure up to 65 bar. Experiments have been performed at the COSMEA test facility at HZDR, which is part of the TOPFLOW Two-Phase Flow facility. Objective of the experimental study was a detailed analysis of the interplay between two-phase flow and heat transfer during steam condensation in an emergency condenser tube. The experimental results are part of a system and CFD code qualification project for passive heat removal systems. The condenser tube resembles a section of a single tube in the KERENA emergency condenser for which integral tests have been performed at Framatome’s INKA test facility in Karlstein, Germany. Beside integral heat flux and condensation rates the experiments at COSMEA deliver high-resolution cross-sectional flow images obtained by X-ray tomography and angularly resolved heat flux through the condenser tube wall. Accompanying CFD simulations have been carried out with ANSYS CFX and a new consistent model for wall and direct contact condensation.

Keywords: KERENA; passive decay heat removal; high-pressure steam condensation; computed tomography; heat flux measurement; CFD modeling

  • Contribution to proceedings
    Specialists Workshop on Advanced Instrumentation and Measurement Techniques for Experiments related to Nuclear Reactor Thermal Hydraulics and Severe Accidents, 22.-25.10.2019, Livorno, Italien
  • Lecture (Conference)
    Specialists Workshop on Advanced Instrumentation and Measurement Techniques for Experiments related to Nuclear Reactor Thermal Hydraulics and Severe Accidents, 22.-25.10.2019, Italien, Livorno

Publ.-Id: 29456

Ultrafast X-ray CT imaging for hydrodynamic investigations of gas-liquid two-phase flow in centrifugal pumps

Schäfer, T.; Neumann-Kipping, M.; Bieberle, A.; Bieberle, M.; Hampel, U.

Gas entrainment into centrifugal pumps decreases pump performance and may raise safety issues, e.g. through insufficient cooling. Although there is some phenomenological knowledge in form of correlations between operating parameters and pump performance a further understanding via direct observation of the gas-liquid mixture was so far not possible. In this paper, we demonstrate the capability of ultrafast X-ray computed tomography (UFXCT) to disclose gas-liquid two-phase flow dynamics in the impeller region of a centrifugal pump mockup. Experiments were performed for gas injection at impeller speeds between 1300 rpm and 1600 rpm. We analyzed the time-resolved X-ray images with respect to the gas distribution and compared them with time-averaged image data of a real pump obtained earlier with gamma-ray tomography.

Keywords: centrifugal pump; gas-liquid two-phase flow; ultrafast X-ray computed tomography

Related publications

  • Open Access Logo Journal of Fluids Engineering - Transactions of the ASME 142(2020)4, 041502
    Online First (2019) DOI: 10.1115/1.4045497


Publ.-Id: 29455

Flow morphology and heat transfer analysis for high-pressure steam condensation in an inclined tube part II: Numerical investigations

Moonesi Shabestary, A.; Bieberle, A.; von der Cron, D.; Ding, W.; Krepper, E.; Lucas, D.; Hampel, U.

In this part of the paper, we introduce and discuss the numerical investigation of two-phase flow and heat transfer during steam condensation inside an inclined tube. For that we developed and employed a three-dimensional two-phase computational fluid dynamics model in ANSYS CFX which comprises a consistent heat transfer model that considers wall condensation and direct contact condensation. Wall condensation is covered by a new subgrid model for the thin liquid film. For modelling of the heat transfer on the steam-liquid interface, three different heat transfer correlations have been implemented to check their performance. Simulation results were compared with experimental data of the COSMEA facility, which has been documented in part I of this paper. Particular focus was given to the development of the liquid film inside the tube and its effects on the wall heat transfer. Moreover, we compared the CFD simulations with system code simulations performed with the ATHLET submodule of AC².

Keywords: wall condensation; direct contact condensation; wall heat flux; liquid film thickness; CFD modelling; AC²; ATHLET


Publ.-Id: 29454

Thermodynamic and structural aspects of the aqueous uranium(IV) system – hydrolysis vs. sulfate complexation

Lehmann, S.; Foerstendorf, H.; Zimmermann, T.; Patzschke, M.; Bok, F.; Brendler, V.; Stumpf, T.; Steudtner, R.

The aquatic species of U(IV) in acidic aqueous solution in the presence of sulfate was studied in the micromolar range by a combined approach of optical spectroscopies (UV/vis and mid-IR), quantum-chemical calculations (QCC), and thermodynamic modelling. The number of species occurring in solution within the pH range 0–2 was assessed by decomposition and fitting of photometric spectra using HypSpec and Geochemist’s Workbench software. Single component spectra of U⁴⁺, UOH³⁺, USO₄²⁺ and U(SO₄)₂ were obtained and extinction coefficients ελ have been calculated to be 58.8, 19.2, 47.6 and 40.3 L mol ⁻ ¹ cm ⁻ ¹, respectively. Complex formation constants of two U(IV) sulfate species and the first hydrolysis species UOH³⁺ in infinite diluted solution were determined by thermodynamic modelling to be log β⁰₁₀₁ = 6.9 ± 0.3, log β⁰₁₀₂ = 11.8 ± 0.5 and log β⁰₁₁₀ = − (0.36 ± 0.1), respectively. No further U(IV) sulfate and hydrolysis species were observed under the prevailing conditions. Molecular structural information of the sulfate species was derived from vibrational spectra and QCC exhibiting a predominant monodentate coordination of the sulfate ions.

Keywords: speciation; absorption; photometry; vibrational spectroscopy; complex formation constant; DFT


Publ.-Id: 29453

Flow morphology and heat transfer analysis during high-pressure steam condensation in an inclined tube part I: Experimental investigations

Bieberle, A.; Moonesi Shabestary, A.; Geißler, T.; Boden, S.; Beyer, M.; Hampel, U.

In this paper, experimental investigations on the flow morphology and heat transfer in a single steam condenser tube are presented, which were performed at the thermal hydraulic test facility COSMEA (COndensation test rig for flow Morphology and hEAt transfer studies). This facility has been setup to study the interrelation of condensation heat transfer with two- phase flow in an isolated single condenser tube that is cooled by forced convection. Studies have been performed for elevated pressures up to 65 bar at saturation conditions and for inlet steam mass flow of up to 1 kg/s and different inlet steam qualities. The wall heat flux is measured with distributed heat flux probe and global condensation rates have been obtained from integral heat and mass balances. As a unique feature the cross-sectional phase distribution has been studied via X-ray computed tomography. The data is going to be used for the validation of numerical simulations with 1D ATHLET and 3D CFD codes as presented in the second part of this paper.

Keywords: condensation heat transfer; heat exchangers; two-phase flow; heat flux; X-ray tomography; passive safety systems

Related publications


Publ.-Id: 29452

Modeling of passive heat removal systems: A review with reference to the Framatome BWR reactor KERENA : Part II

Manthey, R.; Viereckl, F.; Moonesi Shabestary, A.; Zhang, Y.; Ding, W.; Lucas, D.; Schuster, C.; Leyer, S.; Hurtado, A.; Hampel, U.

Passive safety systems are an important feature of currently designed and constructed nuclear power plants. They operate independent of external power supply and manual interventions and are solely driven by thermal gradients and gravitational force. This brings up new needs for performance and reliably assessment. This paper provides a review on fundamental approaches to model and analyze the performance of passive heat removal systems exemplified for the passive heat removal chain of the KERENA boiling water reactor concept developed by Framatome. We discuss modelling concepts for one-dimensional system codes such as ATHLET, RELAP and TRACE and furthermore for computational fluid dynamics codes. Part I dealt with numerical and experimental methods for modelling of condensation inside the emergency condenser and on the containment cooling condenser. This second part deals with boiling and two-phase flow instabilities.

Keywords: Passive heat removal systems; Condensation; System codes; CFD; Emergency condensers; Containment cooling condensers; Two-phase flow instabilities


Publ.-Id: 29451

Modelling of passive heat removal systems: A review with reference to the Framatome BWR reactor KERENA :Part I

Moonesi Shabestary, A.; Viereckl, F.; Zhang, Y.; Manthey, R.; Lucas, D.; Schuster, C.; Leyer, S.; Hurtado, A.; Hampel, U.

Passive safety systems are an important feature of currently designed and constructed nuclear power plants. They operate independent of external power supply and manual interventions and are solely driven by thermal gradients and gravitational force. This brings up new needs for performance and reliably assessment. This paper provides a review on fundamental approaches to model and analyze the performance of passive heat removal systems exemplified for the passive heat removal chain of the KERENA boiling water reactor concept developed by Framatome. We discuss modelling concepts for one-dimensional system codes such as ATHLET, RELAP and TRACE and furthermore for computational fluid dynamics codes. Part I deals with numerical and experimental methods for modelling of condensation inside the emergency condensers and on the containment cooling condenser while part II deals with boiling and two-phase flow instabilities.

Keywords: Passive heat removal systems; condensation; 1D Codes; CFD; emergency condensers; containment cooling condensers

Publ.-Id: 29450

Polarization-dependent near-field phonon nanoscopy of oxides: SrTiO₃, LiNbO₃, and PbZr₀.₂Ti₀.₈O₃

Wehmeier, L.; Lang, D.; Liu, Y.; Zhang, X.; Winnerl, S.; Eng, L. M.; Kehr, S. C.

Resonant infrared near-field optical spectroscopy provides a highly material-specific response with sub-wavelength lateral resolution of about 10 nm. Here, we provide the near-field response of selected paraelectric and ferroelectric materials, i.e. SrTiO3, LiNbO3, and PbZr0:2Ti0:8O3, showing resonances in the wavelength range from 13.0 to 15.8 µm. We investigate these materials using scattering scanning near-field optical microscopy (s-SNOM) in combination with a tunable midinfrared free-electron laser (FEL). Fundamentally, we demonstrate that phonon-induced resonant near-field excitation surprisingly is possible for both p- and s-polarized incident light, a fact that is of particular interest for the nanoscopic investigation of anisotropic and hyperbolic materials. Moreover, we show that near-field spectroscopy, as compared to far-field techniques, bears substantial advantages such as lower penetration depths, stronger confinement, and a high spatial resolution. The latter permits the investigation of minute material volumes, e.g. with nanoscale changes in crystallographic structure, which we prove here via near-field imaging of ferroelectric domain structures in PbZr0.2Ti0.8O3 thin film.

Keywords: Near-field microscopy; ferroelectrica


Publ.-Id: 29449

Direct Correction of Residual Symmetric Aberrations in Electron Holograms of Weak Phase Objects

Kern, F.; Linck, M.; Wolf, D.; Niermann, T.; Arora, H.; Alem, N.; Erbe, A.; Gemming, S.; Lubk, A.

Thin TEM specimen are regarded as weak objects (WPO), if the amplitude variation of the electron wave by the specimen can be neglected and the phase modulation is very small (≪π). Large classes of topical materials can be described in this approximation, such as most 2D materials, organic semiconductor materials or biological specimen. Due to the lack of amplitude (and hence intensity) contrast, conventional TEM (CTEM) investigations on WPOs are commonly performed under a certain defocus, which transfers part of the phase information to the recorded intensity. This intermixing contrast transfer from amplitude to phase and vice versa is commonly described by the phase contrast transfer function (PCTF), while the non-mixing contrast transfer for amplitude and phase is referred to as amplitude contrast transfer function (ACTF). Due to the transfer gap in the PCTF, the CTEM contrast transfer at low spatial frequencies is degraded in defocused images of WPOs (Fig. 1). By employing electron holography, however, both amplitude and phase of the electron wave can be reconstructed without a transfer gap. Having the whole wave information also enables the a-posteriori correction of geometric aberrations as it was already proposed in D. Gabor’s seminal paper from 1948 [1]. The realization of his idea, however, remains challenging in the absence of additional knowledge about the sample, due to the lack of a criterion for a successful aberration correction.

Keywords: electron holography; ERC; density-functional calculations; all-electron; 2D materials

  • Lecture (Conference)
    Microscopy Conference 2019, 01.-06.09.2019, Berlin, Deutschland
  • Microscopy and Microanalysis 25(2019)S2, 98-99
    DOI: 10.1017/S1431927619001223

Publ.-Id: 29448

Simulation of STM images and spectroscopy of single nitrogen-doped molecules with 5-7 membered rings on Au(111) surfaces

Nikipar, S.; Ryndyk, D. A.; Gemming, S.; Moresco, F.; Cuniberti, G.; Frauenheim, T.

We consider STM images and spectroscopy (STS) of molecules on metal surfaces. We combine DFT based atomistic tight-binding model (DFTB approach) with Green function technique, which offers a framework to consider tip, molecule and surface as one integrated system and taking into account the tip geometry. Besides, it captures the interference and interaction effects. This approach can be applied for the investigation of finite-voltage effects and describe the high-energy molecular transport states. It allows to simulate quantitatively the I(V) current-voltage spectroscopy curves and dI/dV maps in both constant current and constant height modes. We applied our methods to nitrogen-doped molecules with 5-7 membered rings on Au(111) surface and showed that the electronic properties of molecules are strongly influenced by formation of azulene-motifs. We developed the integrated open software suite for quantum nanoscale modeling (TraNaS OpenSuite, for convenient calculations of large-scale molecular nanosystems on metal surfaces.

Keywords: molecular electronics; STM; conductance calculations; density-functional tight binding

  • Poster
    DPG Frühjahrstagung, 31.03.-05.04.2019, Regensburg, Deutschland

Publ.-Id: 29447

Electron Transport through single Mn-salen molecule: Theoretical Study

Lokamani, M.; Kilibarda, F.; Sendler, T.; Zahn, P.; Mortensen, M.; Gothelf, K. V.; Erbe, A.; Gemming, S.

Metal-salen complexes, formed by the coordination of a metal cation and a N,N’-bis(salicylidene)ethylenediamine-based ligand, are promising candidates for molecular electronics, because of possible modulations of transport channels using different metal cations. One such candidate is Mn-salen complex.

Here, we first explore the electronic structure of single molecules using wave function (MS-CASSCF) and density-functional (DFT+U) methods. We then employ the non-equilibrium Green’s function (NEGF) technique to study electron transport through single molecules attached to gold electrodes under finite bias. We explore various docking configurations for the single molecule between the gold electrodes.

A comparison with experimental coupling constants and energy levels, obtained using mechanically controllable break junction (MCBJ) technique is also presented.

Keywords: molecular electronics; NEGF; density-functional theory; Hartree-Fock; ab-initio; complete active space; multiconfigurational approach; transport calculation

  • Lecture (Conference)
    DPG Frühjahrstagung, 31.03.-04.05.2019, Regensburg, Deutschland

Publ.-Id: 29446

Statistical studies of random silicon-germanium alloys using electronic structure calculations

Roscher, W.; Fuchs, F.; Wagner, C.; Schuster, J.; Gemming, S.

Random alloys are relevant for many applications. One example is silicon-germanium which is used for high frequency devices like heterojunction-bipolar transistors. We therefore investigate the electronic structure of Si1−xGex alloys in the entire composition range 0≤ x≤ 1. For our study we use density functional theory in combination with bulk models of the alloys. To describe the band gap precisely we use the pseudopotential projector shift method as implemented in QuantumATK 18.06.

We perform a random generation of Si1−xGex structures to get statistical distributions of the electronic properties. After optimizing the structure we evaluate the band structure by averaging equivalent directions in the Brillouin zone.

The mean of the band gap is in good agreement with experimental reference data. We also demonstrate wide variations of the band gap, which are in the range of about 10 %. Further properties, such as the lattice constant and the formation energy are studied as well. Finally, we investigated also the impact of additional carbon dopants in the silicon-germanium alloy.

Keywords: Silicon nanowires; germanium nanowires; random alloys; Monte-Carlo; grand canonical potential simulations; entropy corrections; density functional calculations; mixing enthalpy; mixing entropy

  • Poster
    DPG Frühjahrstagung, 31.03.-05.04.2019, Regensburg, Deutschland

Publ.-Id: 29445

Understanding the formation of interlayer excitons in the case of MoS2 on GaSe.

Wagner, C.; Rahaman, M.; Zahn, D. R. T.; Gemming, S.

The fabrication of hybrid van-der-Waals heterostructures of two-dimensional nano materials is an emerging field of study: The (weak) electronic interaction between two layers is often reasonably described by a perturbation of the physical effects of the isolated layers, such as electrostatic doping and screening of intralayer excitons. However, it turns out that this picture of the weak interaction is not exhaustive in terms of optical properties: the formation of bound excitons from electrons of one layer and the holes from another layer yields the formation of interlayer excitons. These states are measured experimentally by photoluminescence and photocurrents, e.g. in the case of MoS2 on GaSe due to type-II band alignment.

This contribution elucidates the conditions for the formation of interlayer excitons from a first-principles point of view. For this, first-principles studies of a minimal test system are conducted. One perspective is then to predict these states as a function of the heterostack in order to specifically taylor efficient solar cells.

Keywords: densit-function calculations; 2D materials; interlayer exciton; exciton; Bethe-Salpeter; two-particle excitations; 2D heterostructure

  • Lecture (Conference)
    DPG Frühjahrstagung, 31.03.-05.04.2019, Regensburg, Deutschland

Publ.-Id: 29444

Understanding the electron transport through NiSi2-Si interfaces

Fuchs, F.; Gemming, S.; Schuster, J.

Metal-semiconductor interfaces are of huge importance for applications and can be found in various field-effect transistors. We study the interface between NiSi2 and silicon on the basis of density functional theory and the NEGF formalism. Different crystal orientations and strain states are investigated systematically.

We focus on the tunneling phenomena of carriers through the Schottky contact at the interface, which are crucial for the on-current in transistors. The on-current is found to be strongly dependent on strain and orientation. It will be shown that the height of the Schottky barrier determines the tunneling current. However, not all changes in the current can be traced back to the barrier height. The modification of the electronic structure matter as well, which can be modeled based on the effective mass of the tunneling carriers. We have also extracted work functions of the isolated materials which we relate to the extracted Schottky barrier heights. It will be shown that the Schottky-Mott model fails for this material system. Better approaches will be discussed in our contribution.

Keywords: one-dimensional transport; density-functional theory; electronic structure; reconfigurable electronics; RFET; silicon nanowires; nickel silicides; 1D contacts

  • Invited lecture (Conferences)
    International Workshop "Correlations and Transport in one-dimensional structures", 04.-07.07.2019, Dresden, Deutschland
  • Lecture (Conference)
    DPG-Frühjahrstagung, 31.03.-05.04.2019, Regensburg, Deutschland
  • Invited lecture (Conferences)
    Seminar Series on Topical Problems in Theoretical Physics, 20.03.2019, London, U.K.

Publ.-Id: 29443

Modeling the interaction of magnetically capped colloidal particles

Neumann, M.; Gemming, S.; Steinbach, G.; Erbe, A.

Colloidal self-assembly bears significant potential for the bottom-up fabrication of advanced materials and micromechanical structures. A wide range of particles with different types of anisotropy have been recognized as promising precursors for controlled structure engineering. Here, we concentrate on particles that interact via polar fields, which are intrinsically anisotropic. More specifically, we focus on the assembly of micron-sized silica spheres which are partly covered by a thin ferromagnetic layer with an out-of-plane magnetic anisotropy. To study assemblies of such magnetic particles, we introduce a simple two-parameter model: The extended magnetization distribution is approximated by a current-carrying coil enclosed inside a hard sphere. The far field of that current reproduces the stray field of a point dipole model, the near field reflects an extended magnetization. Such a model employs only two parameters to describe the shape of the magnetization distribution: The radius and the position of the coil inside the sphere. We present stable assemblies as a function of both parameters. In the limit of very small coils the analytical solution for two particles with shifted point dipoles is correctly reproduced. By increasing the radius of the coil, we reproduce experimentally observed particle arrangements not covered by models based on single shifted dipoles.

Keywords: colloid; Janus particle; self-assembly; model potential; soft matter

  • Poster
    Frühjahrstagung der Deutschen Physikalischen Gesellschaft, 31.03.-05.04.2019, Regensburg, Deutschland

Publ.-Id: 29442

Characterization of irradiation-induced microstructure in reactor pressure vessel steels

Ulbricht, A.; Bergner, F.; Keiderling, U.

SANS contributed significantly to the understanding of the behaviour of reactor pressure vessel (RPV) steels exposed to irradiation with fast neutrons. It allows macroscopically representative, statistically reliable and robust measures of size, volume fraction and number density of nmsized solute clusters to be obtained. In particular, the use of the ferromagnetic properties of the matrix allows, under certain assumptions, the exact determination of the scattering contrast and thus the absolute volume fraction. The lower detection limit in terms of volume fraction is typically about 0.005%. The A-ratio, that is the total-to-nuclear scattering ratio, can be used as one-parameter signature of the mean composition of irradiation-induced clusters. Major limitations of SANS are related to the uncertainty of the scattering contrast (cluster composition, magnetism) and to the lower detection limit. Especially because of the incoherent scattering contribution of different iron isotopes, the lower detection limit is approximately 0.5 nm in terms of radius. The unirradiated reference condition of a RPV steel exhibits a high scattering background essentially caused by different sizes of carbides and should be carefully subtracted from the investigated neutron-damaged condition.
In the present work we give an overview about major influence factors on irradiation-induced microstructural changes. Increase of neutron exposure gives rise to an increase of the volume fraction of solute clusters. This susceptibility is essentially determined by the existing alloying elements and impurities. Cu-rich precipitates are the dominant type of nanofeatures in Cubearing steels (Cu> 0.1wt%) and Mn-Ni-(Si) precipitates or their nonequilibrium precursors are the dominant type of nanofeatures in low-Cu, Mn-Ni-alloyed ferritic materials. The size of clusters remains small and does not exceed a radius of 4 nm. In recent years, research was focussed on the transferability from accelerated irradiations to real operation conditions of materials in a power reactor, for instance the effect of neutron flux on irradiation-induced damage. Here, SANS results show a clear trend. The size distribution of low flux condition is shifted towards larger radii. The effect of neutron flux on the volume fraction of irradiationinduced clusters is not so obvious. There seems to be a trend that the cluster volume fraction decreases at increasing flux. Here, the detection limits of SANS (very small clusters and/or reduced scattering contrast) and the uncertainties of the irradiation conditions possibly hide an explicit flux dependence. Differences in the A-ratio were not observed for flux pairs of one and the same material. Thus, no significant changes of cluster composition appear at different fluxes.
Strong and robust correlations between SANS-based characteristics of irradiation-induced clusters, such as (the square-root of) volume fraction and irradiation-induced changes of mechanical properties, such as Vickers hardness, yield stress or brittle/ductile transition temperature are confirmed.

Keywords: small-angle neutron scattering; irradiation-induced clusters; reactor pressure vessel steel

  • Poster
    canSAS XI workshop, 08.-11.07.2019, Freising, Deutschland

Publ.-Id: 29440

Flux effect on RPV materials

Ulbricht, A.

The effect of neutron flux on the irradiation-induced microstructure and mechanical behaviour is one of the still open issues for the scientific community both for RPV steels and internals. In the case of RPV steels, more and statistically more reliable microstructural data are needed, in particular for low-Cu RPV steels irradiated up to high fluence. Within SOTERIA, suitable pairs of low-Cu RPV steels irradiated at different flux up to the same levels of fluence were identified.
This deliverable D2.1 reports about the effect of neutron flux on the neutron-irradiation-induced microstructure of RPV base and weld materials. The main methods applied are small-angle neutron scattering (SANS), positron lifetime spectroscopy (PAS), transmission electron microscopy (TEM) and atom probe tomography (APT).
Using these methods, a number of different kinds of irradiation-induced nanofeatures were detected. These comprise dislocation loops, vacancies, sub-nm vacancy clusters, solute atom clusters and segregated dislocations. Loops are insufficient in number density and vacancy clusters are too small to contribute significantly to the irradiation-induced changes of the mechanical properties, but play a role in the overall evolution of the irradiated microstructures. Solute atom clusters are decisive for irradiation hardening.
SANS and APT indicate a common trend that an increasing flux gives rise to smaller sizes and higher number densities of solute atom clusters. APT additionally shows that the clusters are more dilute at higher flux. The counteracting effects of flux on size and number density of solute atom clusters partly compensate each other and, therefore, rationalize the relative insensitivity of the mechanical properties to the neutron flux.

Keywords: reactor pressure vessel steel; low Cu; microstructure; neutron irradiation; flux effect; vacancy/solute cluster

  • Lecture (others)
    SOTERIA Final Workshop, 25.-27.06.2019, Miraflores de la Sierra, Spain

Publ.-Id: 29439

Eulerian-Eulerian two-fluid model for laminar bubbly pipe flows: validation of the baseline model

Liao, Y.; Upadhyay, K.; Schlegel, F.

In the present paper, an Euler-Euler two-fluid model combined with the baseline model, which is a set of closures for the interfacial momentum and turbulence transfer, is validated against experimental data for low Reynolds number bubbly flows in vertical pipes. The model has already been validated for high Reynolds number pipe flows and bubble columns in the previous work (Liao et al., 2019, Chem. Eng. Sci. 202, 55-69). To further substantiate the k-omega SST model with consideration of bubble-induced source included in the baseline model, it is of interest to examine it for low Reynolds number pipe flows, where the bulk is laminar and the transition to turbulence is induced sorely by the agitation of bubbles. Simulations are configured and carried out in the open source CFD code OpenFOAM for eight test cases. Each of them has a different combination of gas and liquid volumetric flow rates. The numerical results are then compared with the experimental data taken from the literature. The comparison is based on different parameters including air void fraction, mean bubble velocity, mean liquid velocity, turbulent kinetic energy and Reynolds shear stress.
Although, mostly, confirming results with the experimental data are presented but further improvement of the model for turbulent transition as well as inter-phase momentum transfer is necessary. Reliable prediction of velocity profile in single-phase and extremely sparse bubbly flow cases is shown, and the phase distribution in fully-developed cases is well captured. In addition to the bulk Reynolds and void fraction, the pipe-to-bubble size ratio is found to have definite influence on the laminar-turbulent transition.

Keywords: Baseline model; Bubbly flows; Bubble-induced turbulence; Low-Re (Reynolds) flows; OpenFOAM


Publ.-Id: 29438

Benchmarking of CFD modelling closures for two-phase turbulent bubbly flows

Colombo, M.; Rzehak, R.; Fairweather, M.; Liao, Y.; Lucas, D.

Eulerian-Eulerian computational fluid dynamic models are used in the prediction of multiphase gas-liquid flows in nuclear reactor thermal hydraulics and in many other chemical and process engineering applications. The modelling approach, based on the concept of interpenetrating continua, allows the calculation of complex and large-scale industrial flows with a relatively limited computational load. However, interfacial transfer processes need to be entirely modelled through numerous closure relations. A large number of different optimized closure sets are available, each often showing remarkable accuracy, but generally only over a few experimental data sets. This specificity makes it difficult to compare the overall accuracy of the models and obstructs the development of more general and robust approaches. In this paper, the bubbly flow models developed at the University of Leeds and the Helmholtz-Zentrum Dresden - Rossendorf are benchmarked against relevant experiments. These two research groups follow a similar modelling approach, aimed at identifying a single universal set of widely applicable closures. The models, implemented respectively in Star-CCM+ and CFX, are applied to a large selection of bubbly flows in different geometries. The main focus is on the momentum transfer, mainly responsible for the lateral bubble distribution in any flow, and on turbulence closures. Therefore, monodispersed bubbly flows that can be effectively characterized with a single average bubble diameter are selected. Overall, the models are found to be generally reliable and robust, and additional developments towards further improved accuracy, increased generality and the definition of a common unified set of model closures are identified. In future, additional benchmark exercises of this kind will be performed, and potentially the definition of proven sets of reference experiments will be recommended.

Keywords: CFD; bubbly flows; two-fluid model; baseline closure; void distribution; two-phase turbulence

  • Contribution to proceedings
    18th International Topical Meeting on Nuclear Reactor Thermal Hydraulics (NURETH-18), 18.-23.08.2019, Portland, Oregon, USA

Publ.-Id: 29437

The intermediate filament synemin regulates non-homologous end joining DNA repair upon genotoxic damage in an ATM dependent manner

Deville, S. S.; Vehlow, A.; Förster, S.; Dickreuter, E.; Borgmann, K.; Cordes, N.

Background: Therapy resistance is a great challenge during cancer treatment. A well-known determinant of radiochemoresistance is cell adhesion to extracellular matrix. Targeting focal adhesion proteins (FAPs) has been shown to enhance cancer radiochemosensitivity in various tumor entities. Previous studies demonstrated a functional crosstalk between specific FAPs and DNA repair processes; however, the molecular mechanism remains unsolved. This study aimed to identify alternative FAPs associated with DNA damage repair mechanisms and radioresistance in head and neck squamous cell carcinomas (HNSCC).
Materials and Methods: A novel 3D High Throughput RNAi Screen (3DHT-RNAi-S) using laminin-rich extracellular matrix was established to determine radiation-induced residual DNA double strand breaks (DSBs) and clonogenic radiation survival using UTSCC15 cells expressing pEGFP-53BP1. Validations were performed in 10 3D grown HNSCC cell lines. DNA repair mechanisms, protein expression and kinetics post irradiation were investigated using immuno-fluorescence/-blotting, reporter assays for DSB repair activity and kinase activity profiling (PamGene) upon protein knockdown with/-out X-ray exposure. Protein-protein interactions were determined using immunoprecipitation (IP) and proximity ligation assay.
Results: In the 3DHT-RNAi-S, Synemin emerged as resulted one of the most promising candidates to determine HNSCC cell radiosensitivitysurvival and DNA damage repair. Synemin silencing radiosensitized HNSCC cells, while its exogenous overexpression induced radioprotection. Synemin depletion elicited a 40% reduction in non-homologous end joining activity without affecting other DNA DSB repair mechanisms. In line, ATM, DNA-PKcs and c-Abl phosphorylation as well as Ku70 expression strongly declined in synemin depleted and irradiated cells relative to controls. In kinome analysis, tyrosine kinases showed significantly reduced activity after synemin silencing relative to controls. Furthermore, IP revealed a protein complex formed between synemin, DNA-PKcs and c-Abl. This protein complex dispersed when ATM was pharmacologically inhibited. Using different protein constructs of synemin (ΔLink-Tail, ΔHead-Link, Synemin_301-961, Synemin_962-1565, S1114A and S1159A), the phosphorylation site at the serine 1114 located on the distal portion of synemin´s tail was identified as essential protein-protein interaction site involved in synemin´s function in DNA repair. Using different protein constructs with domain deletions of synemin, the distal portion of synemin´s tail was identified as essential protein site regulating synemin´s function in DNA repair processes.
Conclusions: The 3DHT-RNAi-S provides a robust screening platform for identifying novel targets involved in therapy resistance. Based on this screen and detailed mechanistic analyses, the intermediate filament synemin was discovered as a novel important determinant of DNA repair, tyrosine kinase activity and radioresistance of HNSCC cells. These results fundamentally support the concept of cytoarchitectural elements as co-regulators of nuclear events.further support the concept that DNA repair is regulated by cooperative interactions between nuclear and cytoplasmic proteins.

Keywords: Radioresistance; HNSCC; Synemin

  • Lecture (Conference)
    DeGBS, 23.09.2019, Mannheim, Deutschland

Publ.-Id: 29435

Emerging Noble Metal Aerogels: State of the Art and a Look Forward

Du, R.; Fan, X.; Jin, X.; Hübner, R.; Hu, Y.; Eychmüller, A.

Noble metal aerogels (NMAs), as the most important class of noble metal foams (NMFs), appear as emerging functional porous materials in the field of materials science. Combining the irreplaceable roles of noble metals in certain scenarios, as well as monolithic and porous features of aerogels, NMAs can potentially revolutionize diverse fields, such as catalysis, plasmonics, and biology. Despite profound progress, grand challenges remain in their fabrication process, including the efficient structure control, the comprehensive understanding of the formation mechanisms, and the generality of the fabrication strategies, thus inevitably retarding the material design and optimization. This Perspective focuses on the key progress, especially of the fabrication strategies for NMAs during the last two decades, while other NMFs are also succinctly introduced. Challenges and opportunities are summarized to highlight the unexploited space and future directions in expectation of stimulating the broad interest of interdisciplinary scientists.

Publ.-Id: 29431

Extending the temperature sensing range using Eu3+ luminescence up to 865 K in a single crystal of EuPO4

Sharma, S.; Köhler, T.; Beyer, J.; Fuchs, M.; Gloaguen, R.; Heitmann, J.

The temperature evaluation through the measurement of emission intensities (intensity ratio method) require two distinct bands; one of which is used as a reference, and the emission intensity of other is monitored as a function of a change in temperature. Herein, we report the influence of excitation wavelengths, and a coupling scheme between lanthanoid and defect emission from the host lattice, to extend the temperature sensing range by using a single crystal of europium (III) phosphate. The temperature dependence of emission intensity was studied for different excitation wavelengths: 365 (intraconfigurational 4f2 excitation), 338 (defect excitation), and 254 nm (O2- →Eu3+ charge-transfer excitation), in the temperature range, 293--865 K. We determined the Boltzmann equilibrium among different coupling schemes using a linear regression model to infer that for an excitation at 338 nm wavelength, and evaluating the intensity ratio between defect emission and the Eu3+ 5D0,1 → 7FJ transitions, the temperature sensing range can be extended upto at least 865 K, with relative sensitivity in the range, 0.33-1.94%K-1 (at 750 K). The results showed resolution of < 1 K with an excellent reproducibility, suggesting that the thermometers can be used with high reliability.

Keywords: photoluminescence; Eu3+ doping; temperature sensing; relative sensitivity

  • Physical Chemistry Chemical Physics 21(2019)29, 16329-16336
    Online First (2019) DOI: 10.1039/C9CP03501J

Publ.-Id: 29430

Achieving optimal laser-proton acceleration through multi-parameter interaction control

Obst-Hübl, L.

Relativistic laser-driven plasmas can be the source of energetic proton beams and have received increasing attention due to their high potential as compact and cost-efficient medical particle accelerators for radiation therapy. As such, exploring viable routes to scale the maximum proton energy to the medically relevant regime remains the subject of ongoing efforts in the Field. This endeavor is inherently linked to the discernment and control of seminal aspects of the acceleration process, ranging on vast temporal and spatial ranges due to highly variable plasma densities and laser intensities within one single interaction. This thesis investigates laser-proton acceleration on various physical scales and the influence of realistic laser pulse parameters, to ultimately find an optimum regime for stable proton beam production with highest particle energies. Experimental studies following this objective were primarily conducted at the high-power titanium:sapphire laser system Draco 150 TW at Helmholtz-Zentrum Dresden-Rossendorf (HZDR). Efficient on-demand control of the temporal laser pulse history was established in the form of a plasma mirror filter combined with on-shot temporal pulse contrast characterization based on an advanced spectral interferometry diagnostic. This allowed for experiments with variable pulse contrast, thus providing additional handles for proton source optimization and additionally, extending the selection of applicable interaction targets to lower thicknesses and densities. Studies with novel target technologies such as ultra-thin liquid crystal films and solid hydrogen jets were performed, each at optimized acceleration conditions, resulting in excellent proton beams with high energies and particle numbers that promise to be highly scalable with increasing laser intensities. Elaborate diagnostic suites in combination with numerical simulations delivered an improved picture of the acceleration process, which generally remains difficult to assess experimentally on the microscopic spatial and ultrafast temporal scale. As an important result, the onset of relativistic target transparency was observed for ultra-thin liquid crystal films, an operation regime that may deliver increased proton energies when optimized. Proton acceleration results from the hydrogen jet agreed well with predictive particle-in-cell simulations, thus establishing a test bed for closely linked experimental and numerical studies into advanced acceleration mechanisms, as are for example associated with target transparency. Furthermore, an unexpected proton beam structuring effect was discovered that can play a significant role in experiments with transparent or very small targets. Formerly unrecognized by the community, this effect leads to the extension of spatial and temporal interaction scales beyond the initial proton acceleration in the laser focus, that need to be considered for appropriate interpretation of proton profile signatures.

  • Doctoral thesis
    TU Dresden, 2019
    Mentor: Dr. Karl Zeil
    150 Seiten
    DOI: 10.5281/zenodo.3252952
  • Lecture (others)
    Verteidigungsvortrag, 18.06.2019, Dresden, Deutschland

Publ.-Id: 29429

Investigation of Bubble Plume Oscillations by Euler-Euler Simulation

Fleck, S.; Rzehak, R.

For practical applications the Euler-Euler two-fluid model relies on suitable closure relations describing interfacial exchange processes. An ongoing effort at HZDR has led to a validated set of closures for adiabatic bubbly flows that is applicable under a rather broad range of conditions including flows in pipes and bubble columns. Up to now, however, only flows with stationary mean values have been considered. The present contribution extends the model validation to dynamic flow phenomena by considering a periodically oscillating bubble plume. Consequently, the turbulence model then runs in URANS mode. Literature data for a partially aerated flat rectangular bubble column are used for comparison. In particular, results for the plume oscillation period show good agreement between simulation and experiment.

Keywords: bubble columns; dispersed gas liquid multiphase flow; Euler-Euler two fluid model; closure relations; CFD simulation; model validation

  • Open Access Logo Chemical Engineering Science 207(2019), 853-861
    DOI: 10.1016/j.ces.2019.07.011
  • Lecture (Conference)
    Jahrestreffen der ProcessNet-Fachgruppe „Computational Fluid Dynamics“, 19.-20.03.2019, Frankfirt/Main, Deutschland


Publ.-Id: 29428

Electron transport through NiSi2-Si contacts and their role in reconfigurable field-effect transistors

Fuchs, F.; Gemming, S.; Schuster, J.

A model is presented which describes reconfigurable field-effect transistors (RFETs) with metal contacts, whose switching is controlled by manipulating the Schottky barriers at the contacts. The proposed modeling approach is able to bridge the gap between quantum effects on the atomic scale and the transistor switching. We apply the model to transistors with a silicon channel and NiSi2 contacts. All relevant crystal orientations are compared, focusing on the differences between electron and hole current, which can be as large as four orders of magnitude. Best symmetry is found for the < 110 > orientation, which makes this orientation most advantageous for RFETs. The observed differences are analyzed in terms of the Schottky barrier height at the interface. Our study indicates that the precise orientation of the interface relative to a given transport direction, perpendicular or tilted, is an important technology parameter, which has been underestimated during the previous development of RFETs. Most of the conclusions regarding the studied metal-semiconductor interface are also valid for other device architectures.

Keywords: density functional; nanowire; nanoelectronics; NanoNet; device modeling; interface; silicide; silicon


Publ.-Id: 29427

Organic Iron Complexes Enhance Iron Transport Capacity along Estuarine Salinity Gradients

Herzog, S. D.; Kvashnina, K.; Persson, P.; Kritzberg, E.

Rivers discharge a notable amount of Fe (1.5 x 109 mol yr−1) to coastal waters, but are still not considered important sources of bioavailable Fe to open marine waters. The reason is that the vast majority of riverine Fe is considered to be lost to the sediment due to aggregation during estuarine mixing. Recently however, several studies demonstrate relatively high stability of riverine Fe to salinity induced aggregation, and it has been proposed that organically complexed Fe (Fe-OM) can “survive” the salinity gradient, while Fe (oxy)hydroxides are prone to aggregation and selectively removed. In this study, we directly identified, by X-ray absorption spectroscopy, the occurrence of these two Fe phases across eight boreal rivers and confirmed a significant but variable contribution of Fe-OM in relation to Fe (oxy)hydroxides among river mouths. We further found that that Fe-OM was more prevalent at high flow conditions in spring than at low flow conditions during autumn, and that Fe-OM was more dominant in low-order streams in a catchment than at the river mouth. The stability of Fe to increasing salinity correlated well to the relative contribution of Fe-OM, i.e. confirming that organic complexes promote Fe transport capacity. This study suggests that boreal rivers may provide significant amounts of potentially bioavailable Fe to marine waters beyond the estuary, due to organic matter complexes

Publ.-Id: 29426

Dual-time-point 64Cu-PSMA-617-PET/CT in patients suffering from prostate cancer

Hoberück, S.; Wunderlich, G.; Michler, E.; Hölscher, T.; Walther, M.; Seppelt, D.; Platzek, I.; Zöphel, K.; Kotzerke, J.

Regardless of its high positron energy, 68Ga-labeled PSMA ligands have become standard of care in metabolic prostate cancer imaging. 64Cu, a radionuclide with a much longer half-life (12.7 h), is available for PSMA labeling allowing imaging much later than 68Ga. In this study, the diagnostic performance of 64Cu-labeled PSMA was compared between early and late scans. Sixteen men (median age: 70 y) with prostate cancer in different stages underwent 64Cu-PSMA-617-PET/CT 2 and 22 hours post tracer injection. Pathologic and physiologic uptakes were analyzed for both points of time. Pathologic tracer accumulations occurred in 12 patients. Five patients presented with pathologic uptake in 17 different lymph nodes, two patients showed pathologic bone uptake in nine lesions, and seven patients had pathologic PSMA uptake in eight prostatic lesions. Physiologic uptake of the renal parenchyma, urine bladder, and salivary glands decreased over time, while the physiologic uptake of liver and bowel increased. In the present study, 64Cu-PSMA-617-PET demonstrated to be feasible for imaging prostate cancer for both the primary tumor site and metastases. Later imaging showed no additional, clinically relevant benefit compared with the early scans. At least the investigated time points we chose did not vindicate the additional expenditure.

Keywords: 64Cu; dual time; PET; prostate cancer; PSMA

  • Journal of Labelled Compounds and Radiopharmaceuticals 62(2019)8, 523-532
    Online First (2019) DOI: 10.1002/jlcr.3745


Publ.-Id: 29425

Spin textures and spin waves as seen by x-ray microscopy

Wintz, S.

The investigation of spin-wave phenomena, also referred to as magnonics, plays an important role in present condensed matter research. This holds true, in particular, as spin waves are seen as signal carriers for future spintronic information processing devices, with a high potential to outperform present charge-based technologies in terms of energy efficiency and device miniaturization. Yet a successful implementation of magnonic technology will require the usage and control of spin waves with nanoscale wavelengths. Here, I will show that ferromagnetic spin textures in metallic systems can be used as nanoscale spin-wave emitters and wave guides. In particular, topological spin vortex cores prove to act as efficient and tunable generators for sub-100 nm waves, while domain walls can be utilized as quasi one-dimensional channels for spin-wave propagation and routing. The underlying spin dynamic processes were directly imaged by using time-resolved x-ray microscopy.

  • Invited lecture (Conferences)
    NAP 2019, 15.-20.09.2019, Odessa, Ukraine
  • Invited lecture (Conferences)
    Challenges & Opportunities in X-Ray Microscopy, 11.-15.02.2019, Kreuth (Schloss Ringberg), Deutschland
  • Invited lecture (Conferences)
    SpinS-2019, 02.-04.10.2019, Duisburg, Deutschland

Publ.-Id: 29424

Decoherence of collective motion in warm nuclei

Frauendorf, S.; Petrache, C.; Schwengner, R.; Wimmer, K.

Collective states in cold nuclei are represented by a wave function that assigns coherent phases to the participating nucleons. The degree of coherence decreases with excitation energy above the yrast line because of coupling to the increasingly dense background of quasiparticle excitations. The consequences of decoherence are discussed, starting with the well studied case of rotational damping. In addition to superdeformed bands, a highly excited oblate band is presented a new example of screening from rotational damping. Suppression of pair correlation leads to incoherent thermal M1 radiation, which appears as an exponential spike (LEMAR) at zero energy in the gamma strength function of spherical nuclei. In deformed nuclei a Scissors Resonance appears and LEMAR changes to damped magnetic rotation, which is interpreted as partial restoration of coherence.

Keywords: Collective motion in atomic nuclei; quantal coherence; collective bands; rotational damping; magnetic rotation; thermal M1 radiation; Scissors resonance

Publ.-Id: 29423

ExploreASL: a collaborative effort to process and explore multi-center ASL data

Mutsaerts, H. J.; Petr, J.; Groot, P.; Ingala, S.; Robertson, A.; Vaclavu, L.; Groote, I.; Kuijf, H.; O'Daly, O.; Zelaya, F.; Vandemaele, P.; Wink, A. M.; Kant, I.; Caan, M.; Morgan, C.; de Bresser, J.; Lysvik, E.; Schrantee, A.; Shirzadi, Z.; Kuijer, J. P. A.; Anazodo, U.; Richard, E.; Bokkers, R.; Reneman, L.; Masellis, M.; Achten, E.; Günther, M.; Macintosh, B.; Golay, X.; Hendrikse, J.; Chapell, M.; van Osch, M.; Thomas, D.; de Vita, E.; Bjornerud, A.; Nederveen, A.; Asllani, I.; Barkhof, F.

Arterial spin labeling (ASL) has undergone significant development since its inception; yet, standardized images processing procedures remain elusive. We present ExploreASL, a robust open source ASL image processing pipeline for clinical studies. Initiated through the European COST action ASL network, this joint effort provides integration and analysis of both single- and multi-center datasets across different operating systems. ExploreASL is optimized for both native- and standard-space analyses, and provides visual and automatic quality control on all intermediate and final images, allowing exploration of ASL datasets from multiple perspectives.

  • Contribution to proceedings
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada
    Proceedings of the ISMRM 27th Annual Meeting & Exhibition, 2705
  • Poster
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada

Publ.-Id: 29422

Hemodynamic impairments in asymptomatic unilateral carotid artery stenosis are increased within individual watershed areas

Kaczmarz, S.; Goettler, J.; Petr, J.; Hansen, M. B.; Kufer, J.; Hock, A.; Sorg, C.; Zimmer, C.; Mouridsen, K.; Hyder, F.; Preibisch, C.

Internal carotid-artery stenosis (ICAS) causes complex and not yet well understood physiological impairments, which currently limits treatment decisions. We present multimodal perfusion and oxygenation-related MRI-data from unilateral asymptomatic ICAS-patients and age-matched healthy controls. The major aim was to investigate hemodynamic impairments in ICAS within individually defined watershed areas (iWSA’s) to account for individual vascular configurations. We found statistically significant lateralization of hemodynamic parameters within iWSA’s - strongest in WM of iWSA’s. Therefore, our iWSA-based approach facilitates detection of even subtle hemodynamic changes in ICAS. Furthermore, we detected spatially widespread capillary flow heterogeneity increases which are promising future treatment indicators.

  • Contribution to proceedings
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada
    Proceedings of the ISMRM 27th Annual Meeting & Exhibition, 3246
  • Poster
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada

Publ.-Id: 29421

Recovery of cerebrovascular reactivity after asymptomatic carotid artery stenosis treatment is assessable by Breathhold-fMRI within global watershed areas

Kaczmarz, S.; Goettler, J.; Sollmann, N.; Kufer, J.; Hansen, M. B.; Hock, A.; Sorg, C.; Zimmer, C.; Mouridsen, K.; Hyder, F.; Preibisch, C.; Petr, J.

Asymptomatic unilateral internal carotid-artery stenosis (ICAS) causes complex and currently poorly understood hemodynamic impairments which could possibly improve treatment decisions. Cerebrovascular reactivity (CVR) is an important biomarker of vascular health and can potentially serve to evaluate ICAS-treatment efficacy. We present perfusion MRI-data from a longitudinal study in 16 asymptomatic ICAS-patients before and after treatment plus 17 age-matched healthy controls. We hypothesize that CVR impairments in ICAS and their recovery after treatment can be assessed by Breathhold-fMRI analyzed by a data-driven approach. Our results demonstrate statistically significant CVR impairments within global watershed areas before treatment and significant CVR recovery after treatment.

  • Contribution to proceedings
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada
    Proceedings of the ISMRM 27th Annual Meeting & Exhibition, 0739
  • Lecture (Conference)
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada

Publ.-Id: 29420

Cerebral hypometabolism measured with intravascular T2-prepared tissue relaxation with inversion recovery (T2-TRIR) and pCASL in adults with sickle cell disease

Vaclavu, L.; Petersen, E. T.; Mutsaerts, H. J.; Petr, J.; Majoie, C. B.; Wood, J. C.; Vanbavel, E. T.; Biemond, B. J.; Nederveen, A. J.

Cerebral metabolic rate of oxygen (CMRO2) quantifies the amount of oxygen consumed by the brain, and relies on continuous delivery of nutrients and oxygen via cerebral blood flow (CBF). In sickle cell disease (SCD), CBF is elevated to compensate for chronic anaemia. This study investigates CMRO2 in adults with SCD using T2-prepared tissue relaxation with inversion recovery (T2-TRIR). CBF increased after acetazolamide-induced vasodilation in both groups but CMRO2 reduced even further in SCD patients while it remained stable in controls. Our results suggest that cerebral shunting is exacerbated by high flow conditions.

  • Contribution to proceedings
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada
    Proceedings of the ISMRM 27th Annual Meeting & Exhibition, 0291
  • Lecture (Conference)
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada

Publ.-Id: 29419

A multi-site round robin assessment of ASL using a perfusion phantom

Oliver-Taylor, A.; Hampshire, T.; Mutsaerts, H.-J.; Clement, P.; Warnert, E.; Kuijer, J. P. A.; Baas, K.; Petr, J.; Siero, J. C. W.; Marques, J. P.; Sunaert, S.; Borra, R. J. H.; van Osch, M. J. P.; Golay, X.; Achten, E.

Arterial Spin Labelling shows great promise for perfusion measurements; however, despite numerous volunteer reproducibility studies, comparisons have not been made using a phantom to establish differences due to the acquisition hardware and pulse sequences. We present data from a multi-site study using a perfusion phantom, targeting 3T MRI systems from a single vendor running the same software version.

  • Contribution to proceedings
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada
    Proceedings of the ISMRM 27th Annual Meeting & Exhibition, 2653
  • Poster
    ISMRM 27th Annual Meeting & Exhibition, 11.06.2019, Montreal, Canada

Publ.-Id: 29418

Extra-neurite Perfusion Measurement with Combined Arterial Spin Labeling and Diffusion Weighted MRI

Asllani, I.; Petr, J.; Mutsaerts, H.-J.; Bozzali, M.; Cercignani, M.

Arterial Spin Labeling (ASL) is an MRI method that uses magnetically labeled endogenous water as a tracer for measuring cerebral perfusion in vivo1. The arterial water that is usually 'labeled' at a plane positioned at the base of the brain, perpendicular to the carotids. A post-labeling delay (PLD) is introduced prior to acquisition to allow labeled water to cross the vasculature and perfuse into the tissue1. Because of signal decay due to T1 relaxation, fast acquisition schemes are employed to ensure optimal SNR. Consequently, the spatial resolution of ASL is relatively low (~ 3 x 3 x 6 mm3). As such, the measured blood flow from a given voxel reflects a mixture of signals from gray matter (GM), white matter (WM), and CSF, a phenomenon known as partial voluming (PV)2. To correct for the confounding effects of PV in ASL imaging, an algorithm (PVC) has been developed and already used by several studies2,3. The algorithm is based on GM and WM volume data obtained from the segmentation of the T1w image2, and makes no further distinction between different compartments within the same tissue type. Here, we investigated the potential of PVC ASL to map blood perfusion in the extra-neurite compartment (e.g., soma, glial cells4) and the intra-neurite (comprised of axons and axon terminals4) within the same tissue, independently. We applied the PVC algorithm using compartmental data from a diffusion weighted imaging (DWI) model, referred to as NODDI4. The underlying hypothesis was that the blood flow in the extra- and intra-neurite compartments would vary with the PLD; a short PLD acquisition would increase the flow in the extra-neurite compartment compared to the long PLD for which there should be an increased flow in the intra-neurite compartment instead.
At any given voxel, the blood flow (fT) is given as:
where, VFIn, VFEn, VFIso represent respectively: the intra-neurite, extra-neurite, and non-tissue compartments obtained from NODDI4. By assuming that for each compartment blood flow is constant over a 'kernel', the equation can be re-written in vectorial form to reflect the flow at the voxel in the center of the kernel2, from which then each compartmental flow can be computed using linear regression as detailed in Asllani et al.2..

MRI protocol & image analysis
T1w (MPRAGE), NODDI, and ASL MRI images were obtained on 4 healthy participants (mean age = 44.5 ± 7.4 y, 2 men) a Siemens 3T system. To test the hypothesis that a shorter PLD would increase the signal in the extra-neurite GM compartment, ASL was acquired with a short (200ms) and long PLD (1800ms). Only results from voxels with GM content > 80% are presented.
Fig.1 shows the raw images that were used by the PVC algorithm to extract the flow from each compartment within the GM. For the long-PLD acquisition, average CBF in the extra- and intra-neurite compartments was 76 ± 10 mL/100g*min and 59 ± 8 mL/100g*min, respectively. As hypothesized, for the short-PLD, the CBF signal was contained primarily in the extra-neurite department (118 ± 17 mL/100g*min) with the intra-neurite compartment flow being essentially zero (-0.9 ± 0.6 mL/100g*min). Results from one participant are shown in Fig.2.
Supporting Image: Fig1.jpg
·Fig.1: ‘Raw’ NODDI and ASL images used by the PVC algorithm from one subject. Top row: MPRAGE and VFIn images; middle row: VFEn and VFISO; bottom row: CBF for short PLD (left) and long PLD (right).
Supporting Image: Fig2.jpg
·Fig.2: Top: Extra-neurite GM CBF from short (left) & long (right) PLD acquisitions. Bottom: axial and sagittal views of Intra-neurite CBF for long PLD with areas in blue indicating ~zero signal.

We combined NODDI with PVC ASL MRI to distinguish between blood flow in the extra- and intra-neurite compartments within GM. While these initial results look promising, more work is needed to test the sensitivity of this method and its feasibility for clinical applications. For example, a larger PLD range is needed to test whether the method can be used to detect inter-neurite subcortical flow. If successful, this method could prove invaluable in mapping blood flow with high spatial specificity.

Keywords: Cerebral Blood Flow; Data analysis; fMRI CONTRAST MECHANISMS; MRI

  • Open Access Logo Contribution to proceedings
    Organization for Human Brain Mapping Annual Meeting 2019, 09.-13.06.2019, Rome, Italy
  • Open Access Logo Poster
    Organization for Human Brain Mapping Annual Meeting 2019, 13.06.2019, Rome, Italy


Publ.-Id: 29417

Photoelectrocatalytic degradation of emerging contaminants at WO₃/BiVO₄ photoanodes in aqueous solution

Cristino, V.; Pasti, L.; Marchetti, N.; Berardi, S.; Bignozzi, C. A.; Molinari, A.; Passabi, F.; Caramori, S.; Amidani, L.; Orlandi, M.; Bazzanella, N.; Piccioni, A.; Kesavan, J. K.; Boscherini, F.; Pasquini, L.

WO3/BiVO4 films obtained by electrochemical deposition of BiVO4 over mesoporous WO3 were applied to the photoelectrochemical degradation of selected emerging contaminants (ketoprofen and levofloxacine) in aqueous solutions. The WO3/BiVO4 films in this work are characterized by a mesoporous morphology with a maximum photoconversion efficiency >40% extending beyond 500 nm in Na2SO4 electrolytes.
Oxygen was found to be the dominant water oxidation product (ca. 90% faradaic yield) and no evidence for the photogeneration of OH radicals was obtained. Nevertheless, both 10 ppm levofloxacine and ketoprofen could be degraded at WO3/BiVO4 junctions upon a few hours of illumination under visible light. However, while levofloxacine degradation intermediates were progressively consumed by further oxidation at the WO3/BiVO4 interface, ketoprofen oxidation byproducts, being stable aromatic species, were found to be persistent in aqueous solution even after 15 hours of solar simulated illumination. This indicates that, due to the lower oxidizing power of photogenerated holes in BiVO4 and a different water oxidation mechanism, the employment of WO3/BiVO4 in photoelectrochemical environmental remediation processes is much less universal than that possible with wider band gap semiconductors such as TiO2 and WO3.


  • Secondary publication expected

Publ.-Id: 29416

NH₃‑SCR over V−W/TiO₂ Investigated by Operando X‑ray Absorption and Emission Spectroscopy

Doronkin, D. E.; Benzi, F.; Zheng, L.; Sharapa, D. I.; Amidani, L.; Studt, F.; Roesky, P. W.; Casapu, M.; Deutschmann, O.; Grunwaldt, J.-D.

V−W/TiO2-based catalysts, which are used for the removal of NOx from the exhaust of diesel engines and stationary sources via selective catalytic reduction with NH3 (NH3-SCR), were studied by operando X-ray absorption spectroscopy (XAS) and emerging photon-in/photon-out techniques. In order to minimize the influence of highly X-ray absorbing tungsten and the fluorescence of titanium, we used a high-energyresolution fluorescence setup that is able to separate efficiently the V Kβ1,3 emission lines and additionally allows to record valence-to-core (vtc) X-ray emission lines. High-energy resolution fluorescence-detected XAS (HERFD-XAS) and vtc X-ray emission spectroscopy (vtc-XES) proved to be the only way to perform an operando V K edge X-ray spectroscopic study on industrially relevant V−W/TiO2 catalysts so far. The V−W/TiO2 and V/TiO2 samples synthesized by incipient wetness impregnation and grafting exhibited high activity toward NH3-SCR. Raman spectroscopy showed that they mainly contained highly dispersed, isolated, and polymeric V-oxo species. HERFD-XAS and XES identified redox cycling of vanadium species between V4+ and V5+. With respect to most of the potential NH3 adsorption complexes, density functional theory calculations further showed that vtc-XES is more limited than surface-sensitive techniques such as infrared spectroscopy; hence, a combination of X-ray techniques with IR or similar spectroscopies is required to unequivocally identify the mechanism of NH3-SCR over vanadia-based catalysts.


Publ.-Id: 29415

Synthesis and Characterization of an Epidermal Growth Factor Receptor selective Ru(II) Polypyridyl-Nanobody Conjugate as a Photosensitizer for Photodynamic Therapy

Karges, J.; Jakubaszek, M.; Mari, C.; Zarschler, K.; Goud, B.; Stephan, H.; Gasser, G.

There is currently a surge for the development of novel photosensitizers (PSs) for photodynamic therapy (PDT) since those currently approved are not completely ideal. Among the tested compounds, we have previously investigated the use of Ru(II) polypyridyl complexes with a [Ru(bipy)2(dppz)]2+ and [Ru(phen)2(dppz)]2+ scaffold (bipy = 2,2'-bipyridine; dppz = dipyrido[3,2-a:2′,3′-c]-phenazine, phen = 1,10-phenanthroline). These complexes selectively target DNA. However, since DNA is ubiquitous, it would be of great interest to increase the selectivity of our PDT PSs by linking them to a targeting vector in view of targeted PDT. Herein, we present the synthesis, characterization and in-depth photophysical evaluation of a nanobody containing Ru(II) polypyridyl conjugate selective for the epidermal growth factor receptor (EGFR) in view of targeted PDT. Using ICP-MS and confocal microscopy, we could demonstrate that our conjugate had a high selectivity for the EGFR receptor, which is a crucial oncological target as it is overexpressed and/or deregulated in a variety of solid tumors. However, contrary to expectations, this conjugate was found to not produce reactive oxygen species (ROS) in cancer cells and to be therefore not phototoxic.

Keywords: Bioinorganic Chemistry; Medicinal Inorganic Chemistry; Metal-based drugs; Metals in Medicine; Photodynamic Therapy

Publ.-Id: 29412

Carrier Flotation: State of the Art and its Potential for the Separation of Fine and Ultrafine Mineral Particles

Eckert, K.; Schach, E.; Gerbeth, G.; Rudolph, M.

Critical raw materials (CRMs) are of primary importance for energy storage systems as needed for electromobility. Many mineral deposits which contain CRMs are low-grade ores. To liberate the CRMs, a grinding of the mineral ores to very fine sizes below 20 µm particle size is necessary. However, the present class of industrial flotation plants fail to extract such fine and ultrafine particles. To improve the recovery in fine particle flotation, techniques have been developed which attempt to agglomerate the fine valuable particles into larger aggregates which subsequently can be separated by established technologies such as froth flotation. Carrier flotation is one of these techniques. The present work reviews the state of the art of this technique for the recovery of fines and ultrafines.

Keywords: Flotation; Fine particles; Carrier Flotation


  • Secondary publication expected

Publ.-Id: 29411

Multidimensional characterization of separation processes – Part 1: Introducing kernel methods and entropy in the context of mineral processing using SEM-based image analysis

Schach, E.; Buchmann, M.; Tolosana Delgado, R.; Leißner, T.; Kern, M.; van den Boogaart, K. G.; Rudolph, M.; Peuker, U. A.

An alternative method for the particle tracking approach for scanning electron microscopy-based image analysis is introduced, using kernel density estimates instead of discrete bins. This allows for information that is more robust. Uncertainties of the data are assessed using the bootstrap resampling method. The presented methodology enables the calculation of multidimensional partition curves, which can be used for a detailed analysis of separation processes. It has been found that the statistical entropy is a helpful tool to evaluate the separation efficiency of these partition maps. The methodology was applied to a density separation process of a cassiteritebearing skarn ore from the Hämmerlein deposit in the Erzgebirge region in Germany, which serves as a case study. A Sepro™ Falcon concentrator was utilized for the density separation.

Keywords: Multidimensional characterization; Partition curve; Separation process; Mineral processing; Kernel density estimation; Entropy; Bootstrap resampling


  • Secondary publication expected

Publ.-Id: 29410

Uncertainty assessment in particle tracking processing models of cassiterite in complex skarn ores

Schach, E.; Buchmann, M.; Tolosana Delgado, R.; Kern, M.; Leißner, T.; Möckel, R.; van den Boogaart, K. G.; Rudolph, M.; Peuker, U. A.

An alternative method for the particle tracking approach for SEM-based image analysis is introduced, using kernel density estimates instead of discrete bins. This allows to obtain more robust information. Therefore, the bandwidth adjustment for the kernels is of special importance. Uncertainties of the data are assessed using the bootstrap resampling method. The mentioned methodology enables for the calculation of multidimensional partition curves, which can be used for a detailed analysis of separation processes. The measure of the entropy is used to evaluate the separation efficiency of the partition maps. A density separation process, using a falcon separator and a dry magnetic separation process, using a drum type separator serve as case studies for the described methodology. As feed material for the separation processes a cassiterite bearing skarn ore from the Pöhla deposit in the Erzgebirge region in Germany is used.

  • Lecture (Conference)
    Procemin-Geomet 2018, 28.-30.11.2018, Santiago, Chile

Publ.-Id: 29409

Oil assisted column flotation of a cassiterite-bearing complex skarn ore from the ore mountains, Germany

Schach, E.; Buchmann, M.; Leistner, T.; Kern, M.; Peuker, U. A.; Rudolph, M.

In this study, the flotation characteristics of a cassiterite-bearing fine-grained and complex skarn ore from a deposit in the Ore Mountains is investigated. The tests are performed using an oil-assisted column flotation approach to process very fine ore fractions and avoid losses of cassiterite into the tailings. First, process parameters are obtained for a finely ground artificial mixture of quartz, magnetite and cassiterite, simulating the real ore. Thereby, magnetite is used, as iron oxides can have a detrimental effect on the flotation due to a similar flotation behavior. In addition, they can act as a source of multivalent ions, which are known to reduce the concentration of collector molecules, active for flotation. Based on the results, selected parameters are further tested for cassiterite skarn ore from the Hämmerlein deposit including a pre-conditioning and a water exchange step to remove ionic contaminants. The process response is analyzed in detail by XRF (X-ray fluorescence) and MLA (mineral liberation analysis) to get a better understanding of the behavior of the single ore components. Sulfosuccinamate type surfactant is utilized as the collector, emulsifier and to reduce the froth destabilization through nonpolar oil. Sodium hexafluorosilicate is added as the depressant.

Keywords: Complex cassiterite-bearing skarn ore; Oil-assisted column flotation; Sulfosuccinamate collector; Water exchange

  • Lecture (Conference)
    IMPC 2018 - 29th International Mineral Processing Congress, 17.-21.11.2018, Moscow, Russian Federation

Publ.-Id: 29408

Density and Susceptibility: Geometallurgical Characterization of a Cassiterite Bearing Complex Skarn Ore From the Ore Mountains, Germany

Buchmann, M.; Schach, E.; Leißner, T.; Tolosana-Delgado, R.; Kern, M.; Krupko, N.; Rudolph, M.; Peuker, U. A.

In mineral processing, density and magnetic susceptibility are two very fundamental properties. For the beneficiation of valuables to saleable concentrates a detailed understanding of these properties is essential. Especially when it comes to the processing of cassiterite, which is the main mineral for tin production, they become highly prominent. Due to the chemically inert character of cassiterite towards most industrial applied leaching agents, density and magnetic separation processes are mainly applied for its beneficiation. To guarantee an optimized utilization of the different operations not only cassiterite but also the different gangue minerals have to be considered.
In this study, a skarn ore is characterized by density and magnetic susceptibility. Therefore, the material was first split into different density classes by heavy liquid separation. The obtained classes were further separated by their susceptibility to finally obtain a density-susceptibility matrix. For this purpose, an isodynamic separator was used. A more detailed characterization of the materials is done via gas pycnometer, magnetic susceptibility balance and vibrating sample magnetometer to estimate the characteristics of density and susceptibility for the various classes. Further, the determination of the chemical assay and the mineral intergrowth by mineral liberation analysis helps to generate a three dimensional data base for detailed characterization of the present ore.
The objective of this study is to estimate potential material streams for a modular processing plant via characterization of the material for the entire deposit by the two afore mentioned characteristic properties. The established multidimensional data matrix, enables predictions for the separation properties of the material and contributes to the characterization of the deposit within the context of geometallurgy.

Keywords: Geometallurgy; susceptibility; density; skarn ore; cassiterite

  • Lecture (Conference)
    MPC 2018 - 29th International Mineral Processing Congress, 15.-21.09.2018, Moscow, Russian Federation

Publ.-Id: 29407

Flotationscharakteristika eines zinnhaltigen Skarnerzes aus der Lagerstätte Hämmerlein im Erzgebirge

Schach, E.; Buchmann, M.; Astoveza, J.; Bremerstein, I.; Kern, M.; Peuker, U. A.; Rudolph, M.

Im Rahmen des AFK-Projektes beschäftigt sich das Helmholtz-Institut Freiberg mit der Aufbereitung feinster Fraktionen eines zinnhaltigen Skarnerzes. Dazu wird in einer gemeinsamen Studie mit der UVR-FIA GmbH und dem Institut für Mechanische Verfahrenstechnik und Aufbereitungstechnik der TU Bergakademie Freiberg die Flotationscharakteristika des Erzes in Abhängigkeit verschiedener, vorhergehender Aufbereitungsmethoden untersucht, um erste Erkenntnisse über geeignete Flotationsreagenzien und Prozessparameter zu erlangen. Bei diesen Methoden handelt es sich um die Dichtetrennung, Magnetscheidung, Sulfidflotation und die Entschlämmung des Aufgabematerials. Da das Aufgabematerial für die Kassiteritflotation noch sehr grobkörnig ist (x80,3 < 250 µm) wurde ebenfalls der Einfluss eines weiteren Zerkleinerungsschrittes zur Verbesserung des Aufschlussgrades betrachtet.
Als Ergänzung zu der von der UVR-FIA GmbH untersuchten Styrolphosphonsäure wurde für die Flotationsversuche, welche im Rahmen dieses Beitrages durchgeführt wurden, das anionaktive Sulfosuccinamat (Aerosol22®) als Sammler verwendet. Zusätzlich wurde MIBC als Schäumer und Natriumhexafluorosilicat als Drücker eingesetzt. Die Flotation erfolgte bei pH 3 in einer Flotationszelle der Firma Outotec® (GTK LabCell™).
Die Proben wurden sowohl mit Röntgenfluoreszenzanalyse als auch mit „Mineral Liberation Analysis“ (MLA) untersucht. Somit war es möglich, das Verhalten der einzelnen Minerale während der verschiedenen Aufbereitungsschritte genauer zu charakterisieren. Besonderes Augenmerk wurde dabei auf die für die Flotation problematische Bestandteile wie zum Beispiel die Chloritgruppenminerale und die Eisenoxide gelegt.
Um den Einfluss von störenden Metallionen auf die Flotation zu bestimmen, wurde für einige Versuche ein Wasserwechsel nach einer Vorkonditionierung mit Natriumhexafluorsilicat durchgeführt. Weiterhin wurden Wasserproben der Versuche entnommen und hinsichtlich der Ionengehalte mittels ICP-OES analysiert.
Im letzten Schritt wurden die einzelnen Aufbereitungsschritte miteinander kombiniert, um Möglichkeiten für ein Fließbild zur Aufbereitung vergleichbarer Erze aufzuzeigen.

  • Lecture (Conference)
    Tagung "Aufbereitung und Recycling", 08.-09.11.2017, Freiberg, Deutschland

Publ.-Id: 29406

The smaller the valuables, the poorer the recovery – Is that always true?

Schach, E.; Leistner, T.; Rudolph, M.

The recovery of valuables in a flotation process is known to depend on the particle size and to drop for very small particles. The lack of floatability of such particle fractions is often objected to poor particle-bubble collision efficiencies due to low inertial energies. We recently showed that very fine valuable particles do float well and that the overall flotation performance depends more on the size of the gangue particles. Those findings are in contradiction to many classic collision models in which the influence of fine gangue particles is neglected. In this study the effect of the fine gangue particles on the flotation process is investigated and discussed in more detail. Therefore flotation tests with different solid concentrations, particle size fractions and different hydrodynamic conditions are conducted, measuring the energy dissipation and analysing the obtained flotation products. In addition, the wettability of the valuables and the gangue particles is characterized.

  • Poster
    Flotation '17, 13.-16.11.2017, Cape Town, South Africa

Publ.-Id: 29405

Floatation characteristics of a cassiterite bearing complex skarn ore from the Ore Mountains, Germany

Buchmann, M.; Schach, E.; Astoveza, J.; Kern, M.; Urs. A., P.; Rudolph, M.

The flotation characteristics of a cassiterite bearing fine grained and complex skarn ore from the Ore Mountain region is investigated. A sulfosuccinamate type collector is used and sodium hexafluorosilicate is added as depressant. The objective of the experiments is a better understanding of the cassiterite flotation performance as influenced by different pre-processing operations as magnetic separation, gravity separation, sulphide flotation and desliming. Therefore, structure and composition of the feed, the different concentrates and the tailings of each process are analysed in detail by XRF and MLA to get a better understanding of the behaviour of the single ore components in the different processing steps. Problematic minerals (e.g. chlorites) have a negative effect on the selectivity of cassiterite flotation. Therefore, particular attention is payed to the behaviour of these minerals during flotation. Furthermore, the effect of the particle size due to the change in liberation on the flotation process is investigated. Three critical factors are found to greatly influence the flotation performance, namely: (1) particle size; (2) Fe oxides content; and (3) ions in the solution.

Keywords: cassiterite flotation; magnetic separation; density separation; fine grinding; desliming; water exchange

  • Poster
    Flotation, 13.11.2017, Cape Town, South Africa

Publ.-Id: 29404

Assessment of flotation kinetics modeling using information criteria; Case studies of elevated-pyritic copper sulfide and high-grade carbonaceous sedimentary apatite ores

Hassanzadehmahaleh, A.; Hoang, D. H.; Stockmann, M.

Despite flotation kinetic modeling is well discussed in the literature, its evaluation from overfitting, the number of model parameters and model complexities have not been adequately addressed. Flotation kinetic behavior of two deposits including an elevated-pyritic (Cu/S=0.21) complex copper sulfide ore and a high-grade carbonaceous sedimentary apatite (P2O5≥25%) ore were investigated. The flotation kinetic experiments were carried out in a mechanically agitated batch flotation cell. Different flotation kinetic models including seven common empirical and initially four mathematical models were applied to the experimental data. In addition to assessment of the goodness of fit (GOF) for each model, a factor of model complexity was considered using advanced statistical techniques (i.e. Bayesian information (BIC), low of iteratedn logarithm (LILC) and Akaike information (AIC) indices). The results confirmed that flotation kinetic modeling significantly depends on the feed type. The empirical models were found more sensitive than the mathematical ones to the ore properties and the mineral types. Furthermore, the mathematical models demonstrated relatively favorable results than the practical models concerning the variation of ore properties due to the consideration of more parameters in the modeling. Finally, it was concluded that the IC indices must be applied to the process of model selection owing to consideration of GOF, the complexity of a model and model consistency. The IC was introduced as a more reliable indicator than the common regression approach for evaluating, sequential ordering and selecting the suitable flotation kinetic models. Further studies are required for model’s generalizability from a statistical point of view.

Keywords: Flotation kinetic modeling; goodness of fit; information criteria; flotation rate constant; Bayesian information

Publ.-Id: 29403

Lift Forces on Solid Spherical Particles in Unbounded Flows

Shi, P.; Rzehak, R.

The present work is concerned with the lift forces acting on particles immersed in an unbounded fluid. Both mechanisms due to rotation of the particle and vorticity of the fluid flow are considered. Focus is on solid spherical particles at Reynolds numbers up to 103 which are relevant for particulate flows in chemical and minerals engineering. A comprehensive review of existing results from analytical, numerical, and experimental studies is given. In particular in the simulation area many new data have appeared in the past 10 years since the earlier review of Loth [AIAA Journal 46 (2008), 801–809]. The available correlations are critically assessed by comparison to data from experiment and direct numerical simulation. Based on the comparison new correlations are proposed and gaps or inconsistencies in the data are identified. The case of wall-bounded flows will be considered in a sequel.

Keywords: lift force; particles; shear flow; particle rotation; correlation

Publ.-Id: 29402

Nanoscale n++-p junction formation in GeOI probed by tip-enhanced Raman spectroscopy and conductive atomic force microscopy

Prucnal, S.; Berencen, Y.; Wang, M.; Georgiev, Y.; Erbe, A.; Khan, M. B.; Böttger, R.; Hübner, R.; Schönherr, T.; Kalbacova, J.; Vines, L.; Facsko, S.; Engler, M.; Zahn, D. R. T.; Knoch, J.; Helm, M.; Skorupa, W.; Zhou, S.

Ge-on-Si and Ge-on-insulator (GeOI) are the most promising materials for the next-generation nanoelectronics that can be fully integrated with silicon technology. To this day, the fabrication of Ge-based transistors with a n-type channel doping above 5 × 1019 cm−3 remains challenging. Here, we report on n-type doping of Ge beyond the equilibrium solubility limit (ne ≈ 6 × 1020 cm−3) together with a nanoscale technique to inspect the dopant distribution in n++-p junctions in GeOI. The n++ layer in Ge is realized by P+ ion implantation followed by millisecond-flashlamp annealing. The electron concentration is found to be three times higher than the equilibrium solid solubility limit of P in Ge determined at 800 °C. The millisecond-flashlamp annealing process is used for the electrical activation of the implanted P dopant and to fully suppress its diffusion. The study of the P activation and distribution in implanted GeOI relies on the combination of Raman spectroscopy, conductive atomic force microscopy, and secondary ion mass spectrometry. The linear dependence between the Fano asymmetry parameter q and the active carrier concentration makes Raman spectroscopy a powerful tool to study the electrical properties of semiconductors.
We also demonstrate the high electrical activation efficiency together with the formation of ohmic contacts through Ni germanidation via a single-step flashlamp annealing process.

Keywords: GeOI; ion implantation; flash lamp annealing; doping; TERS

  • Open Access Logo Journal of Applied Physics 125(2019), 245703
    Online First (2019) DOI: 10.1063/1.5080289


Publ.-Id: 29401

PIConGPU: Predictive Simulations of Laser-Particle Accelerators with Manycore Hardware

Huebl, A.

The presented thesis establishes simulations on modern massively parallel computing hardware to investigate relativistic laser-driven plasmas. The latter are of special interest as they may provide a compact source for energetic ion beams. Computer simulations provide valuable insight into ultrafast plasma processes, evolving in the ultrahigh intensity (I0 ≫ 1018 W/cm2) focus of the ultrashort (𝜏0=30-500 fs) laser pulses driving the interaction. Such simulations require high numerical resolution and full geometric treatment for reliable predictions, which can only be addressed with high-performance computing. The open source particle-in-cell code PIConGPU, which is developed in the framework of this thesis, answers these demands, providing speed and scalability to run on the world's largest supercomputers. PIConGPU is designed with a modular and extensible implementation, allowing to compute on current and upcoming hardware from a single code base. Furthermore, challenges arising for generated data rates, reaching 1 PByte per simulation, are resolved with scalable data reduction techniques and novel workflows, such as interactive simulations.

Numerical studies are performed on two novel targets for laser-proton acceleration with near-critical and mass-limited properties. A micrometer-scale spherical target is explored with realistic temporal laser contrast, providing an interpretation for experimental results collected at the PW-class laser system PHELIX (𝜏0=500 fs pulse length). In this study, 3D modeling with the GPU supercomputer Titan enabled the identification of pre-expansion to near-critical target conditions, which uncovers a regime of volumetric laser-electron interaction generating a highly directed proton beam. Furthermore, a novel cryogenic hydrogen jet target is researched in close collaboration to experiments at the laser system DRACO (𝜏0=30 fs). This target system provides a unique setup for the isolated investigation of multi-species effects and their influence on the generated ion energy distribution. A novel analytical model provides a link between characteristic modulations in the ion energy spectra and ensemble properties of the microscopic electron distribution. In view of a potential experimental realization, parametric scans are performed confirming the feasibility of the proposed setup.

Keywords: laser-plasma acceleration; modeling; HPC; GPU; laser-ion acceleration; exascale computing; open source; open data

  • Doctoral thesis
    TU Dresden, 2019
    Mentor: Prof. Dr. Ulrich Schramm
    171 Seiten
    DOI: 10.5281/zenodo.3266820
  • Lecture (others)
    Dissertationsverteidigung, 25.06.2019, Dresden, Deutschland


Publ.-Id: 29400

Joint project: Umwandlungsmechanismen in Bentonitbarrieren - Subproject B: Einfluss von mikrobiellen Prozessen auf die Bentonitumwandlung

Matschiavelli, N.; Drozdowski, J.; Kluge, S.; Arnold, T.; Cherkouk, A.

Concerning the deep geological disposal of high-level radioactive waste (HLW), bentonite can be used because of its high swelling capacity and its low hydraulic conductivity as geo-technical barrier and buffering material in between the waste-containing canister (technical barrier) and the surrounding host rock (geological barrier). There are still many gaps in process understanding of bentonite transformations, especially in dependence of different temperatures and pore waters. Within the joint-project UMB (“Umwandlungsmechanismen in Bentonitbarrieren”), the co-operation partner Gesellschaft für Anlagen- und Reaktorsicherheit (GRS) mbH (Repository Safety Analysis), the University of Greifswald (Institute for Geography and Geology), the Federal Institute for Geosciences and Natural Resources (BGR, section of technical mineralogy), the Technical University of Munich (TUM; chair of theoretical chemistry, quantum chemistry) and the Helmholtz-Center Dresden-Rossendorf (HZDR, Institute of Resource Ecology) are supposed to define criteria which facilitate the selection of suitable bentonites in order to use them in the deep geological repository of high-level radioactive waste. HZDR analyzed two different bentonites (B36 and SD80) regarding their microbial diversity and potential microbial activity. In dependence of repository-relevant parameters (temperature, pore water, presence of substrates), microcosm experiments were set up at the GRS, containing the respective bentonites and Opalinus Clay pore water or cap rock solution, respectively. The long-term batches were incubated one year and two years at different temperatures (25 °C, 60 °C and 90 °C) in gastight bottles. Additionally, HZDR set up B36 short-term microcosms with Opalinus Clay pore water, which incubated for three month at 30 °C with six sampling points monitoring the microbial diversity and geochemical parameters.
After one and two years of incubation at 25 °C, respectively, supplemented SD80 microcosms containing Opalinus Clay pore water showed the formation of black precipitates and fissures as well as the dominance of sulfate-reducing and spore-forming bacteria. The detected genera are able to reduce the present sulfate in order to form hydrogen sulfide. XRF spectroscopy analysis, done at the University of Greifswald, showed a decrease in sulfate concentration in the respective SD80 microcosms, supporting this surveillance. Similar observations were made for the two-year incubations. The microbial diversity of the B36 bentonite raw material is much different from the SD80 bentonite raw material. Similar to the diversity of SD80 bentonite, the microbial community of the B36 bentonite long-term incubations changed with respect to the applied pore water. Spore-forming organisms dominated the set ups which were supplied with Opalinus Clay pore water solution whereas halophilic microorganisms were found in set ups containing diluted cap rock solution. We were also successful in showing the dominance of thermophilic bacteria in Opalinus clay pore water-containing microcosms that incubated at 60 °C for two years. Additionally, we were able to enrich microorganism from Opalinus Clay pore water of both, B36 and SD80 bentonite long-term incubations. Similar to the long-term analysis, substrate-containing B36 short-term microcosms, containing Opalinus Clay pore water, showed also the dominance of spore-forming bacteria after three months of incubation. Furthermore, a slight decrease in lactate-concentration as well as an increase in ferrous iron and acetate-concentration was observed in the respective B36 microcosms. The presence of substrates and mesophilic incubation temperatures of 25 °C or 30 °C, respectively, promoted the growth of “microbial generalists” that are able to exist in a vegetative state. Extreme environmental conditions as elevated temperatures (60 °C) or high-salt concentrations promote the dominance of highly specialized microorganisms. Our data show, that the microbial diversity in the analyzed bentonites and, furthermore, the evolution of the respective microbial communities differs significantly from each other. Since not that much is known about intrinsic extremophilic microorganisms (metabolic activity and potential influence on the bentonite barrier material), our data stress the importance of further microbial investigations in order to prevent and reduce potential risks (e.g. corrosion, mineralogical changes), due to microbial activity within the repository.

  • Open Access Logo Wissenschaftlich-Technische Berichte / Helmholtz-Zentrum Dresden-Rossendorf; HZDR-103 2019
    ISSN: 2191-8708, eISSN: 2191-8716


Publ.-Id: 29398

Making a cool choice: the materials library of magnetic refrigeration

Gottschall, T.; Skokov, K. P.; Fries, M.; Taubel, A.; Radulov, I.; Scheibel, F.; Benke, D.; Riegg, S.; Gutfleisch, O.

The phase-down scenario of conventional refrigerants used in gas-vapor compressors and the demand for environmentally friendly and efficient cooling makes the search for alternative technologies more important than ever. Magnetic refrigeration utilizing the magnetocaloric effect of magnetic materials could be that alternative. However, there are still several challenges to be overcome before we have devices that are competitive with those based on the conventional gas-vapor technology. In this paper we present a rigorous assessment of the most relevant examples of 14 different magnetocaloric material families and compare them in terms of their adiabatic temperature and isothermal entropy change under cycling in magnetic-field changes of 1 and 2 T, criticality aspects and the amount of heat that they can transfer per cycle. The work is based on magnetic, direct thermometric and calorimetric measurements made under similar conditions and in the same devices. Such a wide-ranging study has not been carried out before. This data sets the basis for more advanced modelling and machine learning approaches in the near future.

Publ.-Id: 29397

Multiferroic spin-superfluid and spin-supersolid phases in MnCr2S4

Ruff, A.; Wang, Z.; Zherlitsyn, S.; Wosnitza, J.; Krohns, S.; Krug Von Nidda, H.-A.; Lunkenheimer, P.; Tsurkan, V.; Loidl, A.

Spin supersolids and spin superfluids reveal complex canted spin structures with independent order of longitudinal and transverse spin components. This work addresses the question whether these exotic phases can lead to spin-driven ferroelectricity. Here we report the results of dielectric and pyrocurrent measurements of MnCr2S4 as function of temperature and magnetic field up to 60 T. This sulfide chromium spinel exhibits a Yafet-Kittel type spin structure at low temperatures. As function of external magnetic field, the manganese spins undergo a sequence of ordering patterns of the transverse and longitudinal spin components, which can be mapped onto phases as predicted by lattice-gas models including solid, liquid, super-fluid, and supersolid phases. By detailed dielectric and pyrocurrent measurements, we document a zoo of multiferroic phases with sizable ferroelectric polarization strongly varying from phase to phase. Using lattice-gas terminology, the title compound reveals multiferroic spin-superfluid and spin-supersolid phases, while the antiferromagnetic solid is paraelectric.

Publ.-Id: 29396

Biologische Wege zur Rohstoffsicherung – vom Nobelpreis zum Recycling

Lederer, F.

Im Jahr 1985 entwickelte der Wissenschaftler George P. Smith eine Methode zur Identifizierung von kurzen Eiweißbruchstücken, die gezielt und selektiv ein Zielmaterial binden können. Für diese Methode der Evolution im Reagenzglas, welche auf der Verwendung von Bakteriophagen basiert, erhielt er im Jahr 2018 den Chemienobelpreis. Damals half ihm die Methode, Antikörper für bestimmte Krebszellen zu identifizieren. Die Wissenschaftler des Helmholtz-Instituts Freiberg für Ressourcentechnologie nutzen die Phage Surface Display genannte Methode für die Entwicklung hochspezifischer Bioangeln zum seletiven Recycling von Seltenen Erden aus Elektroschrott.

Keywords: Biotechnologie; Phage Surface Display; Bioangeln

  • Lecture (others)
    Lange Nacht der Wissenschaften 2019 in Dresden, 14.06.2019, Dresden, Deutschland

Publ.-Id: 29395

Metallgewinnung durch Mikrobiologie – Biologisch assistierte Prozesse in der Rohstofftechnologie

Lederer, F.

Präsentation der Arbeitsbereiche Bioflotation, Biosorption und Biolaugung, die in der Abteilung Biotechnologie des HIF Schwerpunktmäßig untersucht werden. Vorstellung der Nachwuchsgruppe BioKollekt

Keywords: Phage Surface Display; BioKollekt; Bioflotation; Biolaugung; Biosorption

  • Lecture (others)
    Lehrveranstaltung Industrielle Mikrobiologie im Fachbereich Technische Mikrobiologie, 24.06.2019, Senftenberg, Deutschland

Publ.-Id: 29394

Fermi surface investigation of the semimetal TaAs2

Butcher, T.; Hornung, J.; Förster, T.; Uhlarz, M.; Klotz, J.; Sheikin, I.; Wosnitza, J.; Kaczorowski, D.

The transversal magnetoresistance associated with the semimetal TaAs2 shows a parabolic field dependence that rises unrestrictedly to 2800 at 14 T and 1.8 K. Here, we report the results of a comprehensive quantum-oscillation study. Angular-dependent de Haas–van Alphen (dHvA) data were obtained with the method of cantilever-torque magnetometry. These were compared with the results of density-functional theory calculations, which predict a Fermi surface with two kinds of electron pockets, as well as two types of hole pockets. Only the electron pockets could be xperimentally verified, whereas no evidence for the hole pockets is present in the measured dHvA frequencies.


Publ.-Id: 29393

Fermi surface studies of the skutterudite superconductors LaPt4Ge12 and PrPt4Ge12

Bergk, B.; Klotz, J.; Förster, T.; Gumeniuk, R.; Leithe-Jasper, A.; Lorenz, V.; Schnelle, W.; Nicklas, M.; Rosner, H.; Grin, Y.; Wosnitza, J.

We report on comprehensive de Haas–van Alphen (dHvA) and electronic band-structure studies of the superconducting skutterudites LaPt4Ge12 (Tc = 8.3 K) and PrPt4Ge12 (Tc = 7.9 K). Both materials show very rich spectra of dHvA oscillations with similar and only slightly varying angular-dependent frequencies. The spectral richness can partly be rationalized by the elaborated electronic band structures resulting in several Fermi surfaces built by six different bands. The effective cyclotron masses of both superconductors lie between about 0.5 and 1.1 times the free-electron mass. Although these values are small, we find moderate mass enhancements between about 2 and 4 when comparing to the calculated masses. Our results evidence the localized character of the 4f electrons in the Pr compound and are in line with an electron-phonon mediated multiband superconductivity, largely identical for both compounds.


Publ.-Id: 29392

Hole compensation effect in III-Mn-V dilute ferromagnetic semiconductors

Xu, C.; Wang, M.; Yuan, Y.; Larkin, G.; Helm, M.; Zhou, S.

A systematic study of hole compensation effect on magnetic properties, which is controlled by defect compensation through ion irradiation, in (Ga,Mn)As, (In,Mn)As and (Ga,Mn)P is represented in this work. In all materials, both Curie temperature and magnetization decrease upon increasing the hole compensation, confirming the description of hole mediated
erromagnetism according to the p -d Zener model. The material dependence of Curie temperature and magnetization versus hole compensation reveals that the manipulation of magnetic properties in III-Mn-V dilute ferromagnetic semiconductors by ion irradiation is strongly influenced by the energy level location of the produced defect relative to the band edges in

Keywords: dilute ferromagnetic semiconductors; the Curie temperature; magnetization; compensation effect; ion irradiation

Publ.-Id: 29391

Presenting Non-Invasive and Fully Acceptable Exploration Technologies - The INFACT Project

Viezzoli, A.; Roffey, S.; Wijns, C.; Fernandez, I.; Blanco Gonzalez, J. M.

Despite its rich history of mining and residual mineral wealth, current conditions within the EU present a number of social, political, legislative, cost, technical and physical obstacles to raw material exploration: obstacles to be overcome by innovation, dialogue, and reform. The Innovative, Non-invasive and Fully Acceptable Exploration Technologies (INFACT) project, within the Horizon 2020 program, will work to mitigate each and every one of these obstacles.
Specific to exploration geophysics, the project will facilitate the development of innovative airborne geophysical and remote sensing technologies (less-invasive than classical exploration methods) that promise to penetrate to new depths, reach new sensitivities and resolve new parameters. The project will also set the EU as a leader on the world stage by establishing permanent infrastructure (reference sites) to drive innovation in the next generation of exploration tools: tools that are cost-effective, designed for EU conditions and its raw materials strategy, and high-performing in terms of minimum environmental impact, social acceptability, and technical performance. These reference sites will provide long-term targets over which successive new technologies can be tested against previous ones.

  • Poster
    2nd Conference on Geophysics for Mineral Exploration and Mining, 09.-12.09.2018, Porto, Portugal
    DOI: 10.3997/2214-4609.201802752

Publ.-Id: 29390

Investigations on potential methods for the long-term monitoring of the state of fuel elements in dry storage casks: recent results

Hampel, U.; Wagner, M.; Schmidt, S.; Fiß, D.; Reinicke, S.; Kratzsch, A.

Until a repository is available in deep geological formations, there is a need in Germany for the safe interim storage of spent fuel elements at the power plant sites. It is assumed that considerable periods of more than 50 years will have to be taken into account. Spent fuel elements are stored in Germany in transport and storage casks of the CASTOR type.
A material-scientific question currently being investigated in depth internationally concerns the long-term integrity of the fuel rod cladding tubes during dry storage and thus the safety during transport to the final repository and during secondary packaging. The absorption of hydrogen in the cladding tube during reactor operation leads to the precipitation of hydrides. If the cladding tube temperature increases during reloading or dry storage, a radial reorientation of the hydrides is conceivable due to the tangential stresses caused by the internal rod pressure. This type of hydride arrangement considerably reduces the brittle fracture toughness. A long-term cladding tube failure is conceivable due to a long-term increase in the internal rod pressure (production of gaseous fission products) and a long-term decrease in the cladding tube temperature (reduction of brittle fracture toughness).
Due to the existing uncertainties with regard to the concrete physical processes, the question arises as to the possibility of monitoring the cask contents. Invasive procedures, such as internal probes, are mainly ruled out for reasons of licensing. On the other hand, the massive construction of the containers with a wall thickness of at least 47 cm on all sides limits the spectrum of non-invasive testing and condition monitoring procedures that can be used. Within the DCS-Monitor project, four non-invasive measuring methods are investigated with regard to their suitability for the condition monitoring of the cask inventory by simulations and experiments. For this purpose, damage scenarios of the cask inventory were assumed in a CASTOR V/19, which were identified on the basis of investigations on damage mechanisms. In the following, the recent investigation results of the project are presented.

  • Contribution to proceedings
    3rd Workshop on Safety of Extended Dry Storage of Spent Nuclear Fuel, 05.-07.06.2019, Garching, Deutschland
  • Lecture (Conference)
    3rd Workshop on Safety of Extended Dry Storage of Spent Nuclear Fuel, 05.-07.06.2019, Garching, Deutschland

Publ.-Id: 29389

Role of the hydroxo group in the coordination of citric acid toward trivalent americium

Tamain, C.; Bonato, L.; Aupiais, J.; Dumas, T.; Guillaumont, D.; Barkleit, A.; Berthon, C.; Solari, P. L.; Ikeda-Ohno, A.; Guilbaud, P.; Moisy, P.

The molecular characterization based on multi-technique approach has led to major highlights on revealing the coordination environment of americium (Am) surrounded by citric acid (H3CitH). The structure of the different complexes at pH 1 and 3 are described. These characterizations are made possible by the comparison of the americium-citric acid system with the americium-tricarballylic acid (one analogue of the citric acid without the alpha-hydroxo group). The structural analyses (Vis spectrophotometry, NMR, EXAFS, TRLFS and capillary electrophoresis) were carried out after the establishment of the speciation distribution diagrams so that the complex percentages in solution are known, allowing to take into account the species repartition for structural analysis data treatment. With this combination of means, it was proved for the 1:1 complex that the hydroxo group is counter intuitively deprotonated and coordinated to the Am(III) at pH 1 as well as two carboxylate functions, whereas at pH 3 the hydroxo is not coordinated and stays protonated allowing the three carboxylate functions to coordinate the metallic cation. Therefore, the hydroxo group affects the Am complexation differently depending on the pHs: the complexation is favored by inductive effect at pH 3, and by direct coordination at pH 1.

Keywords: Americium; citric acid; tricarballylic acid; complexation constants; alpha-hydroxycarboxylate; structure; coordination sphere; EXAFS; NMR; capillary electrophoresis; TRLFS; speciation

Publ.-Id: 29388

Identification of Prime Factors to Maximize the Photocatalytic Hydrogen Evolution of Covalent Organic Frameworks

Ghosh, S.; Nakada, A.; Springer, M.; Kawaguchi, T.; Suzuki, K.; Kaji, H.; Baburin, I.; Kuc, A. B.; Heine, T.; Suzuki, H.; Abe, R.; Seki, S.

Visible-light-driven hydrogen (H2) production from water is a promising strategy to convert and store solar energy as chemical energy. Covalent organic frameworks (COFs) are front runners among different classes of organic photocatalysts. The photocatalytic activity of COFs depends on numerous factors such as the electronic band gap, crystallinity, surface area, exciton migration, stability of transient species, charge separation and transport, etc. However, it is challenging to fine tune all of these factors simultaneously to enhance the photocatalytic activity. Hence, in this report, an effort has been made to understand the interplay of these factors and identify the key factors for efficient photocatalytic H2 production through a structure−property−activity relationship. Careful molecular engineering allowed us to optimize all of the above plausible factors impacting the overall catalytic activities of a series of isoreticular COFs. The present study determines three prime factors: light absorption, charge carrier generation, and its transport, which influence the photocatalytic H2 production of COFs to a much greater extent than the other factors.

Publ.-Id: 29387

Phase Transition Induced Carrier Mass Enhancement in 2D Ruddlesden-Popper Perovskites

Baranowski, M.; Zelewski, S. J.; Kepenekian, M.; Traoré, B.; Urban, J. M.; Surrente, A.; Maude, D. K.; Kuc, A. B.; Booker, E. P.; Stranks, S. D.; Plochocka, P.

The variety of possible ways to tune the optical properties of 2D perovskites is their huge advantage, while at the same time, the mutual dependence between different tuning parameters hinder our fundamental understanding of their properties. In this work, we attempt to address this issue for (CnH2n+1NH3)2PbI4 (with n=4,6,8,10,12) using optical spectroscopy in high magnetic fields up to 67T. Our experimental results, supported by DFT calculations, clearly demonstrate that the reduced mass of the exciton increases by around 30% in the low temperature phase. This is reflected by a 2-3 fold decrease of the diamagnetic coefficient. Our studies shows that the effective mass which is essential parameter for optolectronic device operation can be tuned by the variation of organic spacers and/or moderate cooling achievable using Peltier coolers. Moreover, we show that the complex absorption features visible in absorption/transmission specta track each other in magnetic field providing strong evidence for the phonon related nature of the observed side bands.


Publ.-Id: 29386

Vacancy complexes in nonequilibrium germanium-tin semiconductors

Assali, S.; Elsayed, M.; Nicolas, J.; Liedke, M. O.; Wagner, A.; Butterling, M.; Krause-Rehberg, R.; Moutanabbir, O.

Depth-profiled pulsed low-energy positron annihilation lifetime spectroscopy and Doppler broadening spectroscopy were combined to identify vacancy-related complexes and probe their evolution as a function of Sn content in GeSn epitaxial layers. Regardless of the Sn content in the 6.5-13.0 at.% range, all GeSn samples showed the same depth-dependent increase in the positron annihilation line broadening parameters, relative to that of epitaxial and bulk Ge references thus confirming the formation of open volume defects during growth. The measured average positron lifetimes were found to be the highest (380-395 ps) in the region near the surface and monotonically decrease across the analyzed thickness, but remain above 350 ps. All GeSn layers exhibit average lifetimes that are 20 to 160 ps higher than those recorded for the Ge reference. Surprisingly, these lifetimes were found to decrease as Sn content increases in GeSn layers. These measurements indicate that divacancies are the dominant defect in the as-grown GeSn layers. However, their corresponding lifetime was found to be shorter than in epitaxial Ge thus suggesting that the presence of Sn may alter the structure of divacancies. Additionally, GeSn layers were found to also contain a small fraction of vacancy clusters, which become less important as Sn concentration increases. The interaction and possible pairing between Sn and vacancies have been proposed to explain the reduced formation of larger vacancy clusters in GeSn when Sn content increases.

Keywords: GeSn semiconductor; positron annihilation lifetime spectroscopy; Doppler broadening spectroscopy; vacancy complexes; open volume defects divacancies vacancy clusters


Publ.-Id: 29385

Towards reconfigurable electronics: silicidation of top down fabricated Silicon nanowires

Khan, M. B.; Deb, D.; Kerbusch, J.; Fuchs, F.; Löffler, M.; Banerjee, S.; Mühle, U.; Weber, W. M.; Gemming, S.; Schuster, J.; Erbe, A.; Georgiev, Y.

We present results of our investigations on nickel (Ni) silicidation of top-down fabricated silicon nanowires (SiNWs). Control over the silicidation process is important for the applications of SiNWs in reconfigurable field effect transistors (RFETs). Silicidation is performed using a rapid thermal annealing (RTA) process on the SiNWs fabricated by electron beam lithography (EBL) and inductively coupled plasma (ICP) etching. The effect of variations in crystallographic orientations of SiNWs and different NW designs on the silicidation process is studied. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) are done to study Ni diffusion, silicide phases and silicide-silicon interface. Control over the silicide phase is achieved together with atomically sharp interfaces between the silicide and silicon. We find that {111} interfaces are predominantly formed, which are energetically most favorable according to density functional theory calculations. However, control over the silicide length remains a challenge.

Keywords: Schottky junction; field effect transistors; nickel silicide; annealing

Publ.-Id: 29384

Tunable large field magnetoconductance of ZnO, ZnMnO, and ZnCoO thin films

Vegesna, S. V.; Bürger, D.; Patra, R. K.; Dellith, J.; Abendroth, B.; Skorupa, I.; Schmidt, O. G.; Schmidt, H.

Magnetoconductivity of ten ZnO, Zn1-x Cox O, and Zn1-x MnxO thin films with nominal concentrations of 2.0 at.% and 0.1 at.% of Co2+ and Mn2+ ions, respectively, has been analyzed in the temperature range from 5 K to 200 K in in-plane and out-of-plane magnetic fields up to 6 T. The formation of a highly conducting surface layer can be controlled during thin film deposition, leading to a large variation of the sheet resistance, namely, from 2 × 103 ω /□ to 1 × 10 5 ω/□ at room temperature. Depending on the thickness of the highly conducting surface layer, a single two-dimensional (2D), a single three-dimensional (3D), or a two-dimensional and three-dimensional (2D + 3D) parallel conducting model was chosen to analyze the measured magnetoconductivity of the magnetic ZnO thin films with different electron spins (S = 5 / 2 for Zn 1 - x Mn x O and S = 3 / 2 for Zn1-x Cox O) and with different Landé g -factors (isotropic for 3D Zn1-x Mnx O and 2D Zn1-x Cox O and anisotropic for 2D Zn1-x Mnx O and 3D Zn1-x Cox O).

Publ.-Id: 29383

Fundamentals and Applications of Hybrid LWFA-PWFA

Hidding, B.; Beaton, A.; Boulton, L.; Corde, S.; Doepp, A.; Habib, F. A.; Heinemann, T.; Irman, A.; Karsch, S.; Kirwan, G.; Knetsch, A.; Manahan, G. G.; Martinez De La Ossa, A.; Nutter, A.; Scherkl, P.; Schramm, U.; Ullmann, D.

Fundamental similarities and differences between laser-driven plasma wakefield acceleration (LWFA) and particle-driven plasma wakefield acceleration (PWFA) are discussed.
The complementary features enable the conception and development of novel hybrid plasma accelerators, which allow previously not accessible compact solutions for high quality electron bunch generation and arising applications. Very high energy gains can be realized by electron beam drivers even in single stages because PWFA is practically dephasing-free and not diffraction-limited.
These electron driver beams for PWFA in turn can be produced in compact LWFA stages. In various hybrid approaches, these PWFA systems can be spiked with ionizing laser pulses to realize tunable and high-quality electron sources via optical density downramp injection (also known as plasma torch) or plasma photocathodes (also known as Trojan Horse) and via wakefield-induced injection (also known as WII). These hybrids can act as beam energy, brightness and quality transformers, and partially have built-in stabilizing features. They thus offer compact pathways towards beams with unprecedented emittance and brightness, which may have transformative impact for light sources and photon science applications. Furthermore, they allow the study of PWFA-specific challenges in compact setups in addition to large linac-based facilities, such as fundamental beam–plasma interaction physics, to develop novel diagnostics, and to develop contributions such as ultralow emittance test beams or other building blocks and schemes which support future plasma-based collider concepts.

Keywords: plasma physics; accelerators; electron beams; light sources; photon science


Publ.-Id: 29382

Simulación de una pila PEMFC "air-breathing" utilizando el código OpenFOAM

Weber, N.; Ferreira-Aparicio, P.; Chaparro, A.

The open-source CFD code OpenFOAM is being used to simulate the operation conditions of a proton exchange membrane fuel cell (PEMFC), with an 'air-breathing' cathode. The fuel cell operates with ambient air without additional convective elements. The anode works in dead-end mode using a static H2 pressure of 0.5bar, and with a hydrophilic membrane to allow for the evacuation of liquid water. This mode allows for 100% hydrogen consumption in the electrochemical reaction. This fuel cell type is being developed in CIEMAT and applied to small portable applications where extra weight and volume must be minimised, while maximizing hydrogen utilization. Being originally developed for solid oxide fuel cells, the openFuelCell model is extended to PEMFCs for the first time. It will provide basic knowledge of this special fuel cell configuration, essential characteristics of its performance reflected by the polarization curve, liquid water transport, temperature inhomogeneities, and heat transport.

  • Lecture (Conference)
    Congreso Iberoamericano de Hidrógeno y Pilas de Combustible, 23.10.2019, Madrid, Spanien

Publ.-Id: 29381

Which transition metal atoms can be embedded into two-dimensional molybdenum dichalcogenides and add magnetism?

Karthikeyan, J.; Komsa, H.-P.; Batzill, M.; Krasheninnikov, A. V.

As compared to bulk solids, large surface-to-volume ratio of two-dimensional (2D) materials may open new opportunities for post-synthesis introduction of impurities into these systems by, e.g., vapor deposition. However, it does not work for graphene or h-BN, as the dopant atoms prefer clustering on the surface of the material instead of getting integrated into the atomic network. Using extensive first-principles calculations, we show that counterintuitively most transition metal (TM) atoms can be embedded into the atomic network of the pristine molybdenum dichalcogenides (MoDCs) upon atom deposition at moderate temperatures either as interstitials or substitutional im- purities, especially in MoTe2, which has the largest spacing between the host atoms. We further demonstrate that many impurity configurations have localized magnetic moments. By analyzing the trends in energetics and values of the magnetic moments across the periodic table, we rationalize the results through the values of TM atomic radii and the number of (s + d) electrons available for bonding, and suggest the most promising TMs for inducing magnetism in MoDCs. Our results are in line with the available experimental data and should further guide the experimental effort towards a simple post-synthesis doping of 2D MoDCs and adding new functionalities to these materials.

Keywords: 2D materials; electronic structure calcualtions


Publ.-Id: 29380

Analysing tumour growth delay data from animal irradiation experiments with deviations from prescribed dose

Karsch, L.; Beyreuther, E.; Eger Passos, D.; Pawelke, J.; Löck, S.

Abstract: The development of new radiotherapy technologies is a long-term process, which requires proving the general concept although clinical requirements with respect to beam quality and controlled dose delivery may not yet be fulfilled. Exemplarily, the necessary radiobiological experiments with laser-accelerated ion beams are challenged by fluctuating beam intensities. Based on tumour-growth data and dose values obtained in an in-vivo trial comparing the biological efficacy of laser-driven and conventional Linac electrons [2], different statistical approaches for analysis were compared. In addition to the classical averaging per dose point, which excludes animals with high dose deviations, multivariable linear regression, Cox regression and a Monte-Carlo-based approach were tested as alternatives that include all animals in statistical analysis. The four methods were compared based on experimental and simulated data. All applied statistical approaches revealed a comparable radiobiological efficacy of laser-driven and conventional Linac electrons, confirming the experimental conclusion. However, in the simulation study, significant differences in dose-response were observed by all methods except for the conventional method. Thereby, these statistical approaches may allow for reducing the total number of required animals in future pre-clinical trials.

Keywords: pre-clinical studies; statistical analysis; experimental beams; radiotherapy

Publ.-Id: 29379

Comparative effect of trivalent lanthanides and actinides on a rat kidney cell line

Heller, A.; Acker, M.; Barkleit, A.; Bok, F.; Wober, J.

Exposure to trivalent lanthanides (Ln) and actinides (An) poses a serious health risk to animals and humans. Since both Lan and An are mainly excreted with the urine, we investigated the effect of La, Ce, Eu, and Yb (as representatives of Ln) as well as Am (as representative of An) exposure on a rat renal cell line (NRK-52E) for 8, 24, and 48 h in vitro. Cell viability studies using the XXT assay and fluorescence microscopic investigations were combined with solubility and speciation studies using ICP-MS and time-resolved laser-induced fluorescence spectroscopy (TRLFS). Thermodynamic modeling was applied to predict the speciation of Ln and Am in cell culture medium.
All Ln show a concentration- and time-dependent effect on NRK-52E cells with Ce being the most potent element. Effective Ln concentrations reducing the cell viability to 50 % (EC50 values) range from 340 µM for Ce to 1.1 mM for Eu. In general, light and heavy Ln seem to exhibit a greater effect than middle Ln.
In cell culture medium with 10 % fetal bovine serum (FBS), the Ln are completely soluble and complexed with proteins from FBS. Ln speciation is time-independent. Comparative experiment with Am are ongoing and will reveal analogies and differences in the effect of trivalent Ln and An on rat kidney cells.
The results of this study underline the importance of combining biological, chemical, and spectroscopic methods in studying the effect of Ln and An on cells in vitro and may contribute to the improvement of the current risk assessment for Ln in the human body. Furthermore, they demonstrate that Ln seem to have no effect on rat renal cells in vitro at environmental trace concentrations. Nevertheless, especially Ce has the potential for harmful effects at elevated concentrations observed in mining and industrial areas.

[1] A. Heller, Ecotox. Environ. Safe. 2019, 173.

  • Lecture (Conference)
    GDCh-Jahrestagung der Fachgruppe Nuklearchemie 2019, 25.-27.09.2019, Dresden, Deutschland

Publ.-Id: 29378

Calculation of neutron fluence distribution in components in the reactor vicinity and their validation on experiments as a basis for activity calculations

Barkleit, A.; Konheiser, J.

Due to the “German Energiewende”, all nuclear power plants (NPPs) in Germany will be shut down by the end of 2022. Consequently, the safe and sustainable decommissioning and dismantling of the NPPs will be an important challenge for the next decades.
The aim of the project EMPRADO (“Entwicklung einer Methode zur Pre-Aktivitäts- und Dosisleistungsberechnung von reaktornahen Bauteilen auf Basis von Neutronen-fluenzverteilungen” – “Development of a method for pre-activity and dose rate calculations of components in the reactor vicinity based on neutron fluence distributions”) is to develop a standardized method to calculate the specific and temporal progression of activation for reactor components and near-reactor concrete as well as construction elements based on the power history of a nuclear reactor. A non-destructive early radiological characterization in the region of the reactor core is thus possible, which is required for an optimal planning of the dismantling. This can make a significant contribution to minimize the radioactive waste and the radiation exposure of personnel during the decommissioning.
The exact 3D neutron fluence calculations are carried out by Monte-Carlo simulations using the international widely used program MCNP6. For validation of the calculation results neutron flux measurements on the basis of activation foils (monitors) are carried out at several German NPPs which are still in operation.
The monitors used in this project are thin metal foils (10 × 10 × 0.1 mm) of Ti, Fe, Ni, Cu, Zn, Nb, Pd, In, and Sn. They are placed during the annual revision of the NPP at different construction elements, for instance near the reactor pressure vessel and at the first concrete wall, the biological shield, at different heights. At these positions the monitors remain during one working cycle of the NPP; that is approximately one year. After recovery, the neutron activation products are analyzed qualitatively and quantitatively by gamma spectroscopy and liquid scintillation counting (LSC). The experimentally determined activities are compared with the calculated ones in order to optimize the simulation procedure.
First experimental results of a feasibility study carried out in NPP Grohnde will be presented and compared to the available literature.

  • Poster
    Jahrestagung der Fachgruppe Nuklearchemie, 25.-27.09.2019, Dresden, Deutschland

Publ.-Id: 29377

Curved magnetic thin films: fundamentals and applications

Makarov, D.

Extending 2D structures into 3D space has become a general trend in multiple disciplines, including electronics, photonics, plasmonics and magnetics. This approach provides means to modify conventional or to launch novel functionalities by tailoring curvature and 3D shape. We study 3D curved magnetic thin films and nanowires where new fundamental effects emerge from the interplay of the geometry of an object and topology of a magnetic sub-system [1,2]. On the other hand, we explore the application potential of these 3D magnetic architectures for the realization of mechanically shapeable magnetoelectronics [3] for automotive but also virtual and augmented reality appliances [4,5]. The balance between the fundamental and applied inputs stimulates even further the development of new theoretical methods and novel fabrication/characterization techniques [6-8].

[1] R. Streubel et al., Magnetism in curved geometries. J. Phys. D: Appl. Phys. (Review) 49, 363001 (2016).
[2] D. Sander et al., The 2017 magnetism roadmap. J. Phys. D: Appl. Phys. (Review) 50, 363001 (2017).
[3] D. Makarov et al., Shapeable Magnetoelectronics. Appl. Phys. Rev. (Review) 3, 011101 (2016).
[4] G. S. Cañón Bermúdez et al., Magnetosensitive e-skins with directional perception for augmented reality. Science Advances 4, eaao2623 (2018).
[5] G. S. Cañón Bermúdez et al., Electronic-skin compasses for geomagnetic field driven artificial magnetoception and interactive electronics. Nature Electronics 1, 589 (2018).
[6] R. Streubel et al., Retrieving spin textures on curved magnetic thin films with full-field soft X-ray microscopies. Nature Communications 6, 7612 (2015).
[7] T. Kosub et al., All-electric access to the magnetic-field-invariant magnetization of antiferromagnets. Phys. Rev. Lett. 115, 097201 (2015).
[8] T. Kosub et al., Purely antiferromagnetic magnetoelectric random access memory. Nature Communications 8, 13985 (2017).

Keywords: curvilinear magnetism; flexible magnetoelectronics

  • Invited lecture (Conferences)
    Joint European Magnetic Symposia (JEMS), 26.-30.08.2019, Uppsala, Sweden

Publ.-Id: 29376

Application of Magnetism on Curved Surfaces

Makarov, D.

Extending 2D structures into 3D space has become a general trend in multiple disciplines, including electronics, photonics, plasmonics and magnetics. This approach provides means to modify conventional or to launch novel functionalities by tailoring curvature and 3D shape. We study 3D curved magnetic thin films where new fundamental effects emerge from the interplay of the geometry of an object and topology of a magnetic sub-system. On the other hand, we explore the application potential of these 3D magnetic architectures for the realization of mechanically shapeable magnetoelectronics for automotive but also virtual and augmented reality appliances.

Keywords: flexible magnetoelectronics; virtual reality

  • Invited lecture (Conferences)
    European Forum for Science, Research and Innovation, 24.-25.06.2019, Dresden, Germany

Publ.-Id: 29375

A series of tetravalent Pu, Np, U and Th complexes of a salen type ligand

Radoske, T.; Kaden, P.; Walter, O.; Kloditz, R.; Patzschke, M.; Stumpf, T.; März, J.

Fundamental actinide (An) coordination chemistry is still rather scarcely explored though it can provide a deep insight into the bonding situation and bonding trends across the An series. Characteristic of actinides is their huge variety of possible oxidation states, typically ranging from +II to +VII for early An. A suitable approach to explore fundamental physical-chemical properties of actinides is to study series of isostructural An compounds in which the An possesses the same oxidation state. Changes in e.g. the binding situation or magnetic effects among the An series allow insights into their unique electronic properties mainly originating from the 5f-electrons. The tetravalent actinides (An(IV)) are particularly suitable for this kind of systematic studies, as this is the largest accessible series within the early actinides.
Against this background, we performed the current study focusing on a systematic comparison of isostructural An(IV) complexes of Th, U, Np and Pu with a salen type ligand (H2L).
All syntheses and characterizations are conducted under inert, water-free nitrogen atmosphere. SC-XRD results prove that an isostructural complex series was achieved with a molecular unit where two ligands coordinate tetradentately to the An with all oxygen and nitrogen donor atoms. The resulting eightfold coordination environment exhibits a distorted square antiprismatic coordination geometry around the An center. Moreover, the relevant complexes are characterized in solution by NMR spectroscopy displaying characteristic paramagnetic effects according to the unpaired f-electrons. Interestingly, the paramagnetic contributions to the 1H and 13C NMR chemical shifts reach their maximum with [NpL2], and are drastically lower for [PuL2]. The acquired experimental results are further supported by quantum chemical calculations to study the electronic structure of the complexes.

Keywords: tetravalent actinide complexes; coordination chemistry; paramagnetic effects

  • Lecture (Conference)
    49èmes Journées des Actinides, 14.-18.04.2019, Erice, Italy

Publ.-Id: 29374

Cerebral Oxygen Metabolism Measurements with MRI in Adults with Sickle Cell Disease: PF742

Vaclavu, L.; Petersen, E.; Mutsaerts, H.; Petr, J.; Majoie, C.; Wood, J.; Vanbavel, E.; Nederveen, A.; Biemond, B.

MRI studies have demonstrated a high prevalence of silent cerebral infarcts (SCI) in both children and adults with sickle cell disease (SCD). SCI are associated with cognitive impairment and lesion progression in adults with SCD. Disrupted oxygen transport can contribute to cerebral ischemic lesions, despite the compensatory elevation in cerebral blood flow (CBF) in SCD. Investigating the cerebral metabolic rate of oxygen (CMRO2) may therefore give insight into the hemodynamic etiology of SCI in SCD patients. We hypothesized that CMRO2 is reduced in adult patients with SCD as a result of chronic anemia and that vasodilation can improve CMRO2 by generating an increase in blood and oxygen flow.

  • Open Access Logo Poster
    24th Annual Congress of the European Hematology Association, 13.06.2019, Amsterdam, The Netherlands
  • Open Access Logo Contribution to proceedings
    24th Annual Congress of the European Hematology Association, 13.06.2019, Amsterdam, The Netherlands
    Hemasphere, 324-325
    DOI: 10.1097/01.HS9.0000561252.50212.c6

Publ.-Id: 29373

Using Agile Development Platforms for Continuous Integration, Code Review and Collaboration

Schlegel, F.

The reality of scientific software development is of a more or less agile nature. As such, modern code development platforms such as GitHub or GitLab are a great fit to support this process. With their components (issues, projects, continuous integration, etc.) they match the agile development components, merge request enforce a cross-check for all code changes. While a lot of other development workflows are possible, this talk will present the best practice established for large and small projects at HZDR for using these platforms for software development projects.

  • Lecture (Conference)
    Platform for Advanced Scientific Computing (PASC) Conference 2019, 12.-14.06.2019, Zürich, Schweiz

Publ.-Id: 29372

Synthesis and Reactivity of Tetravalent Actinide Amidinates

Schöne, S.; März, J.; Kaden, P.

A series of tetravalent actinide amidinates was synthesized and characterized in solution and in solid state. Quantum chemical calculations support findings based on bonding analysis. Furthermore the reactivity of the complexes is presented.

  • Lecture (others)
    FENABIUM Projekttreffen März 2019, 27.02.2019, Dresden, Deutschland

Publ.-Id: 29371

Enantiopure Tetravalent Actinide Amidinates – Synthesis and Reactivity

Schöne, S.; Kloditz, R.; März, J.; Kaden, P.; Patzschke, M.; Roesky, P. W.; Stumpf, T.

In contrast to the dominant trivalent state for the lanthanide series (Ln(III)), a wide variety of oxidation states (from II to VII) of actinides (An) makes their chemistry intricate but attractive. Especially the early An thorium (Th), uranium (U), neptunium (Np), and plutonium (Pu) form highly charged cations with the oxidation state +IV (An4+), which are of particular interest for coordination chemistry due to their strong interaction with ligands.
The focus of our investigations lies in the comprehensive characterization of An(IV) complexes with ligands bearing soft donor atoms, such as nitrogen (N), both in the solid state and in solution. The present study focuses particularly on the interaction of An(IV) (Th, U, Np) with N-donor ligands of amidinate type, which could be considered as a simplified model of naturally occurring N-donor organic compounds.
Recently, the trivalent lanthanide complexes with the chiral benzamidine, (S,S)-N,N‘-Bis-(1-phenylethyl)-benzamidine ((S)-HPEBA), have been successfully synthesized.[1,2] Mono- and bis-amidinate complexes of the later lanthanides (Er, Yb, Lu) were obtained using a salt metathesis approach. Only for the larger samarium(III) a homoleptic tris-amidinate was accessible.
We have extended this approach to the tetravalent An, and successfully synthesized the first transuranic amidinate complexes. Moreover, we have obtained the first enantiopure amidinate complexes of An(IV) [AnCl((S)-PEBA)3] (An = Th, U, and Np) as well as the analogous Ce(IV) compound, a chemical analog of An(IV). The tris-amidinate complexes have been structurally characterized in solid state and in solution showing a comparable complex geometry.
Due to the presence of a Cl- ligand in the An coordination sphere, it could be speculated that the complex should be reactive. Thus, the reactivity of the complexes has been demonstrated by successful reduction with potassium graphite to homoleptic trivalent actinide amidinates [An((S)-PEBA)3] (An = U, Np).

  • Lecture (Conference)
    Journées des Actinides 2019, 14.-18.04.2019, Erice, Italien

Publ.-Id: 29370

Comprehensive real space bonding analysis of tetravalent f-element complexes with Schiff-base ligands

Kloditz, R.; Radoske, T.; Patzschke, M.; Stumpf, T.

The contribution of the f-orbitals to chemical bonding leads to the rich chemistry of the actinides. This is in contrast to the lanthanides, where it is known that this contribution is less important. Of special interest is the influence of these orbitals on the bonding character of actinides and lanthanides with organic ligands reflecting natural binding motifs.
This study compares the different bonding behavior of tetravalent actinides and lanthanides with the Schiff base salen (see Fig. 1, left) by means of real-space bonding analysis. Our approach makes use of the quantum theory of atoms in molecules (QTAIM), plots of the non-covalent interactions (NCI) and density differences complemented by natural population analysis (NPA). Especially the local properties at the bond critical points (Fig. 1, right), for instance charge, density, ellipticity and others, can be used to characterize a bond’s order, strength, and covalent contribution. In addition, thermodynamic calculations on the stability of these complexes are presented since the difference in stability is a direct consequence of the different interaction strengths of the f elements.
First results reveal a strong interaction of the actinides, i.e. Th to Pu, with the oxygen of salen characterized by a high electron density concentration between the atoms. In contrast, the interaction between the actinides and the nitrogen of salen is much weaker. The delocalization index, density and Laplacian reveal a significant increase of covalency for Pa to Pu compared to Th and Ce being an indicator of the contribution of the f-electrons. Tetravalent Ce as a lanthanide analogue of Th is expected to show a similar bonding behavior, but, surprisingly, this is not the case for all investigated bonding properties.
Such a detailed analysis of the electronic properties of actinide compounds will help to improve understanding of their behavior in the environment as well as in technical processes and leads to the possibility to predict properties of unknown complexes.

Keywords: Actinides; Quantum chemistry; DFT; Bonding; Covalency

  • Lecture (Conference)
    Journees des Actinides, 14.-18.04.2019, Erice, Italien

Publ.-Id: 29369

Hybrid LWFA–PWFA staging as a beam energy and brightness transformer: conceptual design and simulations

Martinez De La Ossa, A.; Assmann, R. W.; Bussmann, M.; Corde, S.; Couperus Cabadağ, J. P.; Debus, A.; Döpp, A.; Ferran Pousa, A.; Gilljohann, M. F.; Heinemann, T.; Hidding, B.; Irman, A.; Karsch, S.; Kononenko, O.; Kurz, T.; Osterhoff, J.; Pausch, R.; Schöbel, S.; Schramm, U.

We present a conceptual design for a hybrid laserdriven plasma wakefield accelerator (LWFA) to beam-driven plasma wakefield accelerator (PWFA). In this set-up, the output beams from an LWFA stage are used as input beams of a new PWFA stage. In the PWFA stage, a new witness beam of largely increased quality can be produced and accelerated to higher energies. The feasibility and the potential of this concept is shown through exemplary particle-in-cell simulations.
In addition, preliminary simulation results for a proof-of-concept experiment in Helmholtz-Zentrum Dresden-Rossendorf (Germany) are shown.

Keywords: laser plasma accelerator; LWFA; PWFA

Publ.-Id: 29368

Dynamics of Charges in Superlong Blacklight-Emitting CaB2O4:Ce3+ Persistent Phosphor

Sharma, S. K.; Bettinelli, M.; Carrasco, I.; Beyer, J.; Gloaguen, R.; Heitmann, J.

The optical and persistent luminescence properties of CaB2O4:Ce3+ phosphor are presented. The optical emission for excitation in the 250–340 nm wavelength region is dominated by two bands at 365 and 460 nm. Lifetime measurements suggested that the 365 nm emission band is due to interconfigurational Ce3+ 5d → 4f transitions. Upon excitation with a 254 nm UV lamp, a superlong persistent luminescence in the UVA1 region (340–400 nm, blacklight) was observed, lasting for at least 15 h, and with excellent reproducibility, which is perfectly suitable for phototherapy application. The initial-rise method was applied on the thermoluminescence glow curves to determine the trap distribution and trap depth. The results suggest that one distinct trap, with an activation energy of ∼0.52 eV, was solely responsible for the persistent luminescence in the CaB2O4:Ce3+ phosphor. The other traps had a quasi-continuous distribution, with activation energies between 0.56 and 1.15 eV. The proposed persistent luminescence and the thermoluminescence mechanisms are elucidated using experimental parameters obtained from the optical and thermoluminescence results and the theoretically calculated electronic structure of the Ce3+ ion in CaB2O4. The lowest Ce3+ 5d1 level was found to be ∼0.97 eV below the conduction band, and the persistent luminescence/thermoluminescence emission was dominated by the radiative transitions between Ce3+ energy levels, 5d → 2F5/2,7/2.

Keywords: Rare earth luminescence; long persistence; photoluminescence; thermoluminescence; mechanism

Publ.-Id: 29367

Nanoscale modification of one-dimensional single-crystalline cuprous oxide

Das, P.; Raibhar, M. K.; Elliman, R. G.; Möller, W.; Facsko, S.; Chatterjee, S.

In this work we report for the first time a method to modify the surface of Cu2O nanowires in a controllable way and physically weld them into a network form, which contributes to higherelectrical conductivity as well as a strong water-repelling nature. We have used state-of-the-art theoretical calculations to support our experimental observations. We demonstrate how varying the irradiation fluence can modulate the surface and decorate the nanowire with a uniformdistribution of Cu8O nanocrystals due to referential sputtering. While several well studied joining techniques are available for carbon and metal-based nanowires, the same information forceramic nanowires is scarce at present. The current study sheds light into this and a state-of-the art 3D simulation technique predicts most of the modifications including surface modulation, oxygen depletion and welding. The welded network shows higher electrical conductivity than the unwelded assembly. With Cu2O being of p-type the current ion beam joining technique shows a novel path for fabricating p-i-n junctions or solar cell devices through bottom-up approach. Furthermore, we have explored the response of this network to moisture. Our calculation based on density functional theory predicts the hydrophilic nature of individual copper oxide nanowires both before and after irradiation. However, the network shows a strong water-repelling nature, which has been explained quantitatively using the Cassie–Baxter model.

Keywords: copper oxide; superhydrophobic; ion irradiation; nanowire; welding

Publ.-Id: 29366

Ab initio path integral Monte Carlo approach to the static and dynamic density response of the uniform electron gas

Groth, S.; Dornheim, T.; Vorberger, J.

In a recent Letter [T. Dornheim et al., Phys. Rev. Lett. 121, 255001 (2018)] we have presented ab initio results for the dynamic structure factor S(q,ω) of the uniform electron gas for conditions ranging from the warm dense matter regime to the strongly correlated electron liquid. This was achieved on the basis of exact path integral Monte Carlo data by stochastically sampling the dynamic local field correction G(q,ω). In this paper we introduce in detail this reconstruction method and provide several practical demonstrations. Moreover, we thoroughly investigate the associated imaginary-time density-density correlation function F(q,τ). The latter also gives us access to the static density-response function χ(q) and static local field correction G(q), which are compared to standard dielectric theories like the widespread random phase approximation. In addition, we study the high-frequency limit of G(q,ω) and provide extensive results for the dynamic structure factor for different densities and temperatures. Finally, we discuss the implications of our findings for warm dense matter research and the interpretation of experiments.

Keywords: electron gas; warm dense matter; response function; structure factor; local field correction; quantum Monte Carlo


Publ.-Id: 29365

Investigations of the interactions of a Halobacterium isolate with uranium using different microscopic and spectroscopic methods

Hilpmann, S.; Bader, M.; Bachran, M.; Steudtner, R.; Schmidt, M.; Stumpf, T.; Cherkouk, A.

Rock salt formations can serve as potential host rocks for the long-term storage of high-level radioactive waste in a deep geological repository. Haloarchaea are widespread under these highly saline conditions. However, there exists a lack of knowledge about the interactions of these microorganisms with radionuclides especially concerning the chemical speciation. Therefore, the interactions of an extremely halophilic archaeon, Halobacterium sp. GP5 1-1 with uranium, one of the major radionuclides of concern, were investigated in detail. This haloarchaeon was isolated from a German rock salt sample. Different microscopic and spectroscopic techniques were used to get an overall image of the occurring processes on a molecular level.
Time-dependent association experiments with two different U(VI) concentrations were performed, to investigate the interaction kinetics of U(VI) with the cells of the haloarchaeon. The amount of bioassociated U(VI) increased with the incubation time at both concentrations. However, the association process at the lower concentration (10 µM) was much faster than at the higher U(VI) concentration (30 µM). Overall, the association process is not exclusively biosorption, being a passive process and normally finished after a short time of incubation (0 – 2 h) [1].
Scanning electron microscopy coupled with energy-dispersive X-ray absorption spectroscopy indicates different interaction mechanisms of the cells at different U(VI) concentrations. It was found that at a concentration of 10µM U(VI) preferentially biomineralization takes place, whereas biofilm-like structures are formed at a concentration of 30µM.
With the help of time-resolved laser-induced luminescence spectroscopy, different aqueous U(VI) species could be extracted from the supernatant. These species differ slightly in dependence of the U(VI) concentration. In general, the formation of a uranyl-carbonate-complex was observed. This could be the result of microbial released CO2 during the process. In contrast to the higher U(VI) concentration, a phosphate species was formed at a U(VI) concentration of 10 µM.
These findings offer new insights into the microbe-actinide interactions at highly saline conditions relevant to high-level radioactive waste disposal in rock salt formations.

[1] J. R. Lloyd, L. E. Macaskie (2002) in “Interactions of Microorganisms with Radionuclides” (Eds.: M.J. Keith-Roach, F. R. Livens), Elsevier, pp. 313-381

  • Poster
    Jahrestagung der Fachgruppe Nuklearchemie 2019, 25.-27.09.2019, Dresden, Deutschland

Publ.-Id: 29364

Selective leaching of rare earth elements (REEs) from eudialyte concentrate after sulfation and thermal decomposition of non-REE sulfates

Balinski, A.; Atanasova, P.; Wiche, O.; Kelly, N.; Reuter, M.; Scharf, C.

Eudialyte, a sodium rich zirconosilicate, is one of the promising sources for REEs, particularly for HREEs+Y. The key challenge by hydrometallurgical processing is the prevention of silica gel formation and REE separation from resulting multi-element leach solutions. This study deals with the selective leaching of REEs from eudialyte concentrate after sulfation and thermal decomposition of non-REE sulfates. We demonstrate how to select the parameters in each process stage to achieve high yields of REEs and to separate them from Zr⁴⁺(+Hf⁴⁺), Nb⁵⁺, Al³⁺ and Fe³⁺. The best result in terms of the separation and the REE yield was achieved with the following parameters: acid addition: 15 mmol/g; roasting temperature: 750 °C; roasting time: 2 h; pulp density: 25 kg/m³; leaching temperature: 20 °C; leaching time: 24 h; stirring speed: 300 rpm. For sufficient conversion of REEs into sulfates H₂SO₄ was added in excess, approximately twice as high as the acid consumption. Water leaching at high solid/liquid ratios caused decrease in the separation factor and REE losses resulting from formation of double sulfates and gypsum.

Keywords: eudialyte concentrate; rare earth elements; separation; sulfation; selective roasting; thermal stability of sulfates; leaching; silica stability during leaching

Publ.-Id: 29363

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