No evidence of mobile gapless excitations

The search for highly mobile gapless spin excitations in quantum spin liquids (QSL) is currently attracting considerable attention. We examined this specific issue via thermal conductivity measurements on one of the most promising QSL candidates, the organic insulator EtMe₃Sb[Pd(dmit)₂]₂ (dmit-131). We performed heat conduction experiments down to 0.07 K on 8 high-quality single crystals of dmit-131 [1]. In agreement with a parallel study [2] and contrary to other reports [3], our body of data consistently and reproducibly shows the absence of a T-linear contribution to the thermal conductivity of dmit-131 at low temperatures, showing that no spin excitation contribute to the heat transport. Consequently, the spin excitations in dmit-131 are localized and not mobile. Our data further reveal a strongly suppressed phonon conductivity, evidence that the phonons are heavily scattered by localized spin excitations. Comparison with published data on numerous spin-liquid materials shows, in fact, that this is a widespread phenomenon and that it should be considered in any future theory of QSLs.

[1] P. Bourgeois-Hope et al., Phys. Rev. X 9, 041051 (2019)
[2] J.M. Ni et al., Phys. Rev. Lett. 123, 247204 (2019)
[3] M. Yamashita et al., Phys. Rev. B 101, 140407(R) (2020)