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Electronic properties of quasi-two-dimensional molecular conductors $X$[Pd(dmit)$_2$]$_2$ are studied theoretically. We construct an effective model based on the fragment molecular orbital scheme developed recently, which can describe the multi-orbital degree of freedom in this system. The tight-binding parameters for a series of $beta$-type compounds with different cations $X$ are evaluated by fitting to first-principles band calculations. We find that the transfer integrals within the dimers of Pd(dmit)$_2$ molecules, along the intramolecular and intermolecular bonds including the diagonal ones, are the same order, leading to hybridization between different molecular orbitals. This results in charge disproportionation within each molecule, as seen in our previous ab initio study [T. Tsumuraya et al, J. Phys. Soc. Jpn. 82, 033709 (2013)], and also to a revised picture of an effective dimer model. Furthermore, we discuss broken-symmetry insulating states triggered by interaction effects, which show characteristic features owing to the multi-orbital nature. The on-site Coulomb interaction induces antiferromagnetic states with intramolecular antiparallel spin pattern, while electron-lattice couplings stabilize non-magnetic charge-lattice ordered states where two kinds of dimers with different charge occupation arrange periodically. These states showing different spatial patterns compete with each other as well as with the paramagnetic metallic state.
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In molecular-based quantum-spin-liquid candidate EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ with two-dimensional $S$=1/2 triangular lattice, a finite residual linear term in the thermal conductivity, $kappa_0/Tequivkappa/T (T rightarrow 0)$, has been observed and attributed to the presence of itinerant gapless excitations. Here we show that the data of $kappa$ measured in several single crystals are divided into two groups with and without the residual linear term. In the first group with finite $kappa_0/T$, the phonon thermal conductivity $kappa_{ph}$ is comparable to that of other organic compounds. In these crystals, the phonon mean free path $ell_{ph}$ saturates at low temperatures, being limited by sample size. On the other hand, in the second group with zero $kappa_0/T$, $kappa_{ph}$ is one order of magnitude smaller than that in the first group, comparable to that of amorphous solids. In contrast to the first group, $ell_{ph}$ shows a glassy-like non-saturating behavior at low temperatures. These results suggest that the crystals with long $ell_{ph}$ are required to discuss the magnetic excitations by thermal conductivity measurements.
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 systematically derive low-energy effective Hamiltonians for molecular solids $beta^prime$-$X$[Pd(dmit)$_{2}$]$_{2}$ ($X$ represents a cation) using ab initio density functional theory calculations and clarify how the cation controls the inter-dimer transfer integrals and the interaction parameters. The effective models are solved using the exact diagonalization method and the antiferromagnetic ordered moment is shown to be significantly suppressed around the spin-liquid candidate of $X$=EtMe$_{3}$Sb, which is reported in experiments. We also show that both the geometrical frustration and the off-site interactions play essential roles in the suppression of antiferromagnetic ordering. This systematic derivation and analysis of the low-energy effective Hamiltonians offer a firm basis to clarify the nature of the quantum spin liquid found in $beta^prime$-EtMe$_{3}$Sb[Pd(dmit)$_{2}$]$_{2}$.
The crystal-field ground state wave function of CeCu$_2$Si$_2$ has been investigated with linear polarized $M$-edge x-ray absorption spectroscopy from 250mK to 250K, thus covering the superconducting ($T_{text{c}}$=0.6K), the Kondo ($T_{text{K}}$$approx$20K) as well as the Curie-Weiss regime. The comparison with full-multiplet calculations shows that the temperature dependence of the experimental linear dichroism is well explained with a $Gamma_7^{(1)}$ crystal-field ground-state and the thermal population of excited states at around 30meV. The crystal-field scheme does not change throughout the entire temperature range thus making the scenario of orbital switching unlikely. Spectroscopic evidence for the presence of the Ce 4$f^0$ configuration in the ground state is consistent with the possibility for a multi-orbital character of the ground state. We estimate from the Kondo temperature and crystal-field splitting energies that several percents of the higher lying $Gamma_6$ state and $Gamma_7^{(2)}$ crystal-field states are mixed into the primarily $Gamma_7^{(1)}$ ground state. This estimate is also supported by re-normalized band-structure calculations that uses the experimentally determined crystal-field scheme.
Structural, magnetization and heat capacity studies were performed on Ce$_2$(Pd$_{1-x}$Ni$_x$)$_2$Sn ($0 leq x leq 1$) alloys. The substitution of Pd atoms by isoelectronic Ni leads to a change in the crystallographic structure from tetragonal (for $x leq 0.3$) to centered orthorhombic lattice (for $x geq 0.4$). The volume contraction thorough the series is comparable to the expected from the atomic size ratio between transition metal components. The consequent weak increase of the Kondo temperature drives the two transitions observed in Ce$_2$Pd$_2$Sn to merge at $x = 0.25$. After about a 1% of volume collapse at the structural modification, the system behaves as a weakly magnetic heavy fermion with an enhanced degenerate ground state. Notably, an incipient magnetic transition arises on the Ni-rich size. This unexpected behavior is discussed in terms of an enhancement of the density of states driven by the increase of the $4f$-conduction band hybridization and the incipient contribution of the first excited crystal field doublet on the ground state properties.
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