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Register a new userAlgebraic Charge Dynamics of Quantum Spin Liquid b-EtMe3Sb[Pd(dmit)2]2
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Shigeki Fujiyama Dr.
Publication date
2017
fields
Physics
and research's language is
English
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Nuclear spin-lattice (1/T1) and spin-spin (1/T2) relaxation rates of the cation sites of a quantum spin-liquid candidate b-EtMe3Sb[Pd(dmit)2]2 and its deuterated sample are presented. The enhanced 1/T1 of 1H and 2D are well analyzed considering the rotations of methyl- and ethyl-groups of the cation with the activation energies of 200K and 1200K respectively. The 1/T1 and 1/T2 at the Sb site that is located on the 2-fold rotation axis remain active down to the lowest temperature with an algebraic temperature dependence of the correlation time as has been observed in the ac response of the dielectric constants.
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The electronic structure of a quantum spin liquid compound, EtMe3Sb[Pd(dmit)2]2, has been studied with angle-resolved photoemission spectroscopy, together with two other Pd(dmit)2 salts in the valence bond solid or antiferromagnetic state. We have resolved several bands that have negligible dispersions and fit well to the calculated energy levels of an isolated [Pd(dmit)2]2 dimer. EtMe3Sb[Pd(dmit)2]2 being a Mott insulator, its lower Hubbard band is identified, and there is a small gap of ~ 50 meV between this band and the chemical potential. Moreover, the spectral features exhibit polaronic behavior with anomalously broad linewidth. Compared with existing theories, our results suggest that strong electron-boson interactions, together with smaller hopping and on-site Coulomb interaction terms have to be considered for a realistic modeling of the organic quantum spin liquid systems like the Pd(dmit)2 salt.
We present the ultralow-temperature specific heat and thermal conductivity measurements on single crystals of triangular-lattice organic compound EtMe$_3$Sb[Pd(dmit)$_2$]$_2$, which has long been considered as a gapless quantum spin liquid candidate. In specific heat measurements, a finite linear term is observed, consistent with the previous work [S. Yamashita $et$ $al.$, Nat. Commun. {bf 2}, 275 (2011)]. However, we do not observe a finite residual linear term in the thermal conductivity measurements, and the thermal conductivity does not change in a magnetic field of 6 Tesla. These results are in sharp contrast to previous thermal conductivity measurements on EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ [M. Yamashita $et$ $al.$ Science {bf 328}, 1246 (2010)], in which a huge residual linear term was observed and attributed to highly mobile gapless excitations, likely the spinons of a quantum spin liquid. In this context, the true ground state of EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ has to be reconsidered.
We study a spin-orbital model for 4$d^{1}$ or 5$d^{1}$ Mott insulators in ordered double perovskites with strong spin-orbit coupling. This model is conveniently written in terms of pseudospin and pseudo-orbital operators representing multipoles of the effective $j=3/2$ angular momentum. Similarities between this model and the effective theories of Kitaev materials motivate the proposal of a chiral spin-orbital liquid with Majorana fermion excitations. The thermodynamic and spectroscopic properties of this quantum spin liquid are characterized using parton mean-field theory. The heat capacity, spin-lattice relaxation rate, and dynamic structure factor for inelastic neutron scattering are calculated and compared with the experimental data for the spin liquid candidate Ba$_{2}$YMoO$_{6}$. Moreover, based on a symmetry analysis, we discuss the operators involved in resonant inelastic X-ray scattering (RIXS) amplitudes for double perovskite compounds. In general, the RIXS cross sections allow one to selectively probe pseudospin and pseudo-orbital degrees of freedom. For the chiral spin-orbital liquid in particular, these cross sections provide information about the spectrum for different flavors of Majorana fermions.
EtMe$_3$Sb[Pd(dmit)$_2$]$_2$, an organic Mott insulator with nearly isotropic triangular lattice, is a candidate material for a quantum spin liquid, in which the zero-point fluctuations do not allow the spins to order. The itinerant gapless excitations inferred from the thermal transport measurements in this system have been a hotly debated issue recently. While the presence of a finite linear residual thermal conductivity, $kappa_0/T equiv kappa/T (T rightarrow 0)$, has been shown [M. Yamashita {it et al.} Science {bf 328}, 1246 (2010)], recent experiments [P. Bourgeois-Hope {it et al.}, Phys. Rev. X {bf 9}, 041051 (2019); J. M. Ni {it et al.}, Phys. Rev. Lett. {bf 123}, 247204 (2019)] have reported the absence of $kappa_0/T$. Here we show that the low-temperature thermal conductivity strongly depends on the cooling process of the sample. When cooling down very slowly, a sizable $kappa_0/T$ is observed. In contrast, when cooling down rapidly, $kappa_0/T$ vanishes and, in addition, the phonon thermal conductivity is strongly suppressed. These results suggest that possible random scatterers introduced during the cooling process are responsible for the apparent discrepancy of the thermal conductivity data in this organic system. The present results provide evidence that the true ground state of EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ is likely to be a quantum spin liquid with itinerant gapless excitations.
We measured the optical signature of the charge density waves (CDWs) in the multiband conductor TTF[Ni(dmit)2]2 by electronic Raman scattering. At low energies, a hump develops below 60 K. This hump is associated to the amplitude mode of the CDW with an energy around 9 meV. Raman symmetry-resolved measurements show that the CDW amplitude mode is anisotropic and that the CDW can be associated to the band nesting of Ni(dmit)2 chains.
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