Anisotropy and spin-triplet excitions in theS = 1/2 gapped antiferromagnet BaCuSi₂O₆.

BaCuSi₂O₆ (also known as Han Purple Pigment) can be regarded as an almost ideal realization of the S = 1/2 system of weakly-interacting spin dimers with the spin-singlet ground state and gapped excitation spectrum [1]. By application of an external magnetic field the gap can be closed, creating a gas of interacting bosonic spin-triplet excitations (triplons). In BaCuSi₂O₆ this phenomenon can be effectively described in terms of the field-induced Bose-Einstein condensation of triplons [2]. Here, we focus on another interesting phenomenon associated with interacting excited triplets but in the low-field quantum-disordered state. We argue that a fine structure observed in low-temperature EPR spectra of BaCuSi2O6 is a fingerprint of triplet excitations (excitons), which are mobile at low temperatures and getting localized when the temperature is increased. Analyzing the angular dependence of the exciton modes allows us to precisely calculate the zero-field splitting with the triplet state and,correspondingly, the anisotropy parameter, D = 0.07 cm_-1. The proposed procedure can be applied for a large number of S = 1/2 gapped quantum antiferromagnets with dimerized or alternating spin structure and might be of particular importance for studying anisotropy effects in S = 1/2 quantum chains (see for instance [3]). In addition, the temperature dependence of the EPR intensity and linewidth has been measured and discussed. The magnitude of the energy spin gap determined by analyzing the temperature dependence of the integrated signal intensity (¢ = 53 K) is in excellent agreement with data obtained from neutron-scattering measurements [1].
[1] Y. Sasago et al., Phys. Rev. B 55 (1997) 8357.
[2] M. Jaime et al., Phys. Rev. Lett. 93 (2004) 087203.
[3] R.D. Somma and A.A. Aligia, Phys. Rev. B 64 (2001) 024410.