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We found a plateau in the magnitude of the isolated magnetic moments as a function of the anisotropy of the transfer integral (t'/t) in the gapless quantum spin liquid (QSL) phase of an S=1/2 triangular lattice molecular solid X[Pd(dmit)2]2 (dmit = 1,3-dithiole-2-thione-4,5-dithiolate), accomplished by a fine-tuning of t'/t through the mixing of cations, X. In contrast, the magnetic susceptibility at the lowest temperature in the QSL phase parametrized by t'/t evinces an unconventional suppression approaching the quantum phase transition, implying significant critical fluctuations., Comment: 6 pages, 5 figures

We investigated the magnetoresistance and the Hall effect in an organic massless Dirac fermion system $\alpha$-(BETS)$_2$I$_3$ under pressure. The Fermi energy of this system is slightly far away from the Dirac points, and thus the $\nu =1$ quantum Hall state is realized in a low magnetic field at low temperatures. Moreover, the experimental formula for chemical potential as a function of temperature is clarified. We succeeded in detecting the inter-band effects of the magnetic field on the Hall conductivity when the chemical potential passes the Dirac points., Comment: 13 pages, 4 figures

The study of non-s-wave unconventional superconductivities in strongly correlated-electron systems has been a central issue in condensed matter physics for more than 30 years. In such unconventional superconductivities, d-wave Cooper pairing with antiparallel spins has been often observed in various quasi-two-dimensional (quasi-2D) bulk systems. Interestingly, many theories predicted that the triangular lattice causes the d-wave pairing to be unstable and may lead to more exotic pairing such as parallel spin (spin-triplet) pairing. Here we focus on a bulk organic triangular-lattice system in which superconductivity emerges near a nonmagnetic Mott insulating phase. We demonstrate, by using low-power nuclear magnetic resonance (NMR) measurements, that the spin susceptibility of the superconducting state retains the normal state value even deep in the superconducting state. This result indicates the possibility that the material exhibits spin-triplet superconductivity. Our finding will bring insights also into understanding the 2D materials with triangular moire superlattices that are considered also to show unconventional superconductivities near Mott-like insulating states., Comment: 10 pages, 6 figures

We investigated the interlayer magnetoresistance in an organic massless Dirac electron system $\alpha$-(BEDT-TTF)$_2$I$_3$ under pressure. We experimentally demonstrate that the width of the zero mode owing to carrier scattering is much narrower than that of the other Landau levels., Comment: 6 pages, 1 figures

A Dirac electron system in solids mimics a relativistic quantum physics that is compatible with Maxwell's equations, by which we anticipate unified electromagnetic responses. We find a large orbital diamagnetism only along the interplane direction and the nearly temperature-independent conductance of the order of e2/h for the new 2D Dirac organic conductor, a-(BETS)2I3. Distinct from conventional electrons in solids whose nonrelativistic effects bifurcate electric and magnetic responses, the observed orbital diamagnetism scales the electrical conductivity for a wide temperature range. This demonstrates that an electromagnetic duality that is valid only within the relativistic framework is revived in solids.

In a one-dimensional (1D) system with degenerate ground states, their domain boundaries, dubbed solitons, emerge as topological excitations often carrying unconventional charges and spins; however, the soliton excitations are only vital in the non-ordered 1D regime. Then a question arises; how do the solitons conform to a 3D ordered state? Here, using a quasi-1D organic ferroelectric, TTF-CA, with degenerate polar dimers, we pursue the fate of a spin-soliton charge-soliton composite matter in a 1D polar-dimer liquid upon its transition to a 3D ferroelectric order by resistivity, NMR and NQR measurements. We demonstrate that the soliton matter undergoes neutral spin-spin soliton pairing and spin-charge soliton pairing to form polarons, coping with the 3D order. The former contributes to the magnetism through triplet excitations whereas the latter carries electrical current. Our results reveal the whole picture of a soliton matter that condenses into the 3D ordered state., Comment: 5 pages, 4 figures. Supplemental Material is available from K. Sunami

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., Comment: 4 pages, 2 figures; (v2) minor revisions, accepted to PRB Rapid Communication

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., Comment: 6 pages, 4 figures

The thermal conductivity $\kappa$ of the quasi-2D organic spin-liquid candidate EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ (dmit-131) was measured at low temperatures, down to 0.07 K. We observe a vanishingly small residual linear term $\kappa_0/T$, in $\kappa/T$ vs $T$ as $T \to 0$. This shows that the low-energy excitations responsible for the sizeable residual linear term $\gamma$ in the specific heat $C$, seen in $C/T$ vs $T$ as $T \to 0,$ are localized. We conclude that there are no mobile gapless excitations in this spin liquid candidate, in contrast with a prior study of dmit-131 that reported a large $\kappa_0/T$ value [Yamashita et al., Science 328, 1246 (2010)]. Our study shows that dmit-131 is in fact similar to $\kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$, another quasi-2D organic spin-liquid candidate where a vanishingly small $\kappa_0/T$ and a sizeable $\gamma$ are seen. We attribute heat conduction in these organic insulators without magnetic order to phonons undergoing strong spin-phonon scattering, as observed in several other spin-liquid materials., Comment: This revision includes a response to Yamashita's paper [M. Yamashita, Journal of the Physical Society of Japan 88, 083702 (2019)], data on a new sample, two new figures (Figs. 5 and 8), and a Supplementary Material (available upon request)

The electrodynamic response of organic spin liquids with highly-frustrated triangular lattices has been measured in a wide energy range. While the overall optical spectra of these Mott insulators are governed by transitions between the Hubbard bands, distinct in-gap excitations can be identified at low temperatures and frequencies which we attribute to the quantum spin liquid state. For the strongly correlated $\beta^{\prime}$-EtMe$_3$\-Sb\-[Pd(dmit)$_2$]$_2$, we discover enhanced conductivity below $175~{\rm cm}^{-1}$, comparable to the energy of the magnetic coupling $J\approx 250$ K. For $\omega\rightarrow 0$ these low-frequency excitations vanish faster than the charge-carrier response subject to Mott-Hubbard correlations, resulting in a dome-shape band peaked at 100~\cm. Possible relations to spinons, magnons and disorder are discussed.

We report experimental measurements and theoretical analysis of Shubnikov-de Haas (SdH) oscillations in a Dirac cone system: the a-(BEDT-TTF)2I3 organic metal under hydrostatic pressure. The measured SdH oscillations reveal anomalies at high magnetic fields B where the 1/B oscillations periodicity is lost above 7 T. We interpret these unusual results within a theoretical model that takes into account intrinsic distortions of the a-(BEDT-TTF)2I3 Dirac cones such as a parabolic particle-hole asymmetric correction. Others possible causes, such as a cone tilting or a Zeeman effect, are carefully ruled out. The observations are consistent among a-(BEDT-TTF)2I3 samples with different Fermi levels.

The Widom line identifies the locus in the phase diagram where a supercritical gas crosses over from gas-like to a more liquid-like behavior. A similar transition exists in correlated electron liquids, where the interplay of Coulomb repulsion, bandwidth and temperature triggers between the Mott insulating state and an incoherent conduction regime. Here we explore the electrodynamic response of three organic quantum spin liquids with different degrees of effective correlation, where the absence of magnetic order enables unique insight into the nature of the genuine Mott state down to the most relevant low-temperature region. Combining optical spectroscopy with pressure-dependent dc transport and theoretical calculations, we succeeded to construct a phase diagram valid for all Mott insulators on a quantitative scale. In the vicinity of the low-temperature phase boundary, we discover metallic fluctuations within the Mott gap, exhibiting enhanced absorption upon cooling that is not present in antiferromagnetic Mott insulators. Our findings reveal the phase coexistence region and Pomeranchuk-like anomaly of the Mott transition, previously predicted but never observed., Comment: Supplementary information after Acknowledgements

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., Comment: 5 pages, 5 figures

Pressure dependence of the conductivity and thermoelectric power is measured through the Mott transition in the layer organic conductor EtMe3P[Pd(dmit)2]2. The critical behavior of the thermoelectric effect provides a clear and objective determination of the Mott-Hubbard transition during the isothermal pressure sweep. Above the critical end point, the metal-insulator crossing, determined by the thermoelectric effect minimum value, is not found to coincide with the maximum of the derivative of the conductivity as a function of pressure. We show that the critical exponents of the Mott-Hubbard transition fall within the Ising universality class regardless of the dimensionality of the system.

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., Comment: 5 pages, 4 figures

We report the first observation of Shubnikov-de Haas (SdH) oscillations and quantized Hall resistance in the multilayered massless Dirac fermion system $\alpha$-(BEDT-TTF)$_2$I$_3$ with tilted cones. Holes were injected into the thin crystal fixed on a polyethylene naphthalate (PEN) substrate by contact electrification. The detection of SdH oscillations whose phase was modified by Berry's phase $\pi$ strongly suggested that the carrier doping was successful in this system. We succeeded in detecting the quantum Hall effect (QHE) with the steps which is the essence of two dimensional Dirac fermion systems. The number of effectively doped layers was examined to be two in this device. We reveal that the correlation between effective layers plays an important role in QHE., Comment: 11 pages, 4 figures

In Mott insulators, the strong electron-electron Coulomb repulsion prevents metallicity and charge excitations are gapped. In dimensions greater than one, their spins are usually ordered antiferromagnetically at low temperatures. Geometrical frustrations can destroy this long-range order, leading to exotic quantum spin liquid (QSL) states. However, their magnetic ground states have been a long-standing mystery. Here we show that a QSL state in the organic Mott insulator EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ with two-dimensional triangular lattice has Pauli-paramagnetic-like low-energy excitations, which are a hallmark of itinerant fermions. Our torque magnetometry down to low temperatures (30 mK) up to high fields (32 T) reveal distinct residual paramagnetic susceptibility comparable to that in a half-filled two-dimensional metal. This demonstrates that the system is in a magnetically gapless ground state, a critical state with infinite magnetic correlation length. Moreover, our results are robust against deuteration, pointing toward the emergence of an extended `quantum critical phase', in which low-energy spin excitations behave as in paramagnetic metals with Fermi surface, despite the frozen charge degree of freedom., Comment: 7 pages, 3 figures. Published in Nature communication

We present limits on Majoron-emitting neutrinoless double-beta decay modes based on an exposure of 112.3 days with 125 kg of Xe-136. In particular, a lower limit on the ordinary (spectral index n = 1) Majoron-emitting decay half-life of Xe-136 is obtained as T_{1/2}^{0\nu\chi^{0}} > 2.6 x 10^{24} yr at 90% C.L., a factor of five more stringent than previous limits. The corresponding upper limit on the effective Majoron-neutrino coupling, using a range of available nuclear matrix calculations, is < (0.8 - 1.6) x 10^{-5}. This excludes a previously unconstrained region of parameter space and strongly limits the possible contribution of ordinary Majoron emission modes to 0\nu\beta\beta decay for neutrino masses in the inverted hierarchy scheme., Comment: 4 pages, 3 figures (1 figure added). Published version in PRC rapid communication

We have discovered two-dimensional zero-gap material with a layered structure in the organic conductor $\alpha$-(BEDT-TTF)$_2$I$_3$ under high hydrostatic pressure. In contrast to graphene, the electron-hole symmetry is not good except at the vicinity of the Dirac points. Thus, temperature dependence of the chemical potential, $\mu$, plays an important role in the transport in this system. The experimental formula of $\mu$ is revealed. We succeeded in detecting the inter-band effects of a magnetic field on the Hall conductivity when $\mu$ passes the Dirac point., Comment: 5 page, 4 figures

The inter-layer magnetoresistance in a multilayered massless Dirac fermion system, $\alpha$-(BEDT-TTF)$_2$I$_3$, under hydrostatic pressure was investigated. We succeeded in detecting the zero-mode (n=0) Landau level and its spin splitting in the magnetic field normal to the 2D plane. We demonstrated that the effective Coulomb interaction in the magnetic field intensifies the spin splitting of zero-mode Landau carriers. At temperatures below 2K, magnetic fields above several Tesla break the twofold valley degeneracy., Comment: 4 page, 4 figures

We report on the experimental results of interlayer magnetoresistance in multilayer massless Dirac fermion system $\alpha$-(BEDT-TTF)$_2$I$_3$ under hydrostatic pressure and its interpretation. We succeeded in detecting the zero-mode Landau level (n=0 Landau level) that is epected to appear at the contact points of Dirac cones in the magnetic field normal to the two-dimensional plane. The characteristic feature of zero-mode Landau carriers including the Zeeman effect is clearly seen in the interlayer magnetoresistance., Comment: 2 pages, 2 figures

Frequency shifts and nuclear relaxations of 13C NMR of the metal-insulator alternating material, (Me-3,5-DIP)[Ni(dmit)2]2, are presented. The NMR absorption lines originating from metallic and insulating layers are well resolved, which evidences the coexistence of localized spins (\pi_loc) and conduction \pi-electrons. The insulating layer is newly found to undergo antiferromagnetic long range order at about 2.5 K, suggesting emergence of S=1/2 Mott insulator. In the metallic layer, we found significant suppressions of static and dynamical susceptibilities of conduction electrons below 35 K, where antiferromagnetic correlation in the insulating layer evolves. We propose a dynamical effect through strong \pi-\pi_loc coupling between the metallic and insulating layers as an origin of the reduction of the density of states.

The Luttinger surface of an organic metal (TTF-TCNQ), possessing charge order and spin-charge separation, is investigated using temperature dependent angle-resolved photoemission spectroscopy. The Luttinger surface topology, obtained from momentum distribution curves, changes from quasi-2D(dimensional) to quasi-1D with temperature. The high temperature quasi-2D surface exhibits 4$k_F$ charge-density-wave (CDW) superstructure in the TCNQ derived holon band, in the absence of 2$k_F$ order. Decreasing temperature results in quasi-1D nested 2$k_F$ CDW order in the TCNQ spinon band and in the TTF surface. The results establish the link in momentum-space between charge order and spin-charge separation in a Luttinger liquid., Comment: 4 pages, 2 figures

Magnetooptical measurements of several quasi-two-dimensional (q2D) organic conductors, which have simple Fermi surface structure, have been performed by using a cavity perturbation technique. Despite of the simple Fermi surface structure, magnetooptical resonance results show a dramatic difference for each sample. Cyclotron resonances (CR) were observed for q-(BEDT-TTF)2I3 and (BEDT-TTF)3Br(pBIB), while periodic orbit resonances (POR) were observed for (BEDT-TTF)2Br(DIA) and (BEDT-TTF)3Cl(DFBIB). The selection of the resonance seems to correspond with the skin depth for each sample. The effective mass of POR seems to have a mass enhancement due to the many-body effect, while effective mass of CR is independent of the strength of the electron-electron interaction. The scattering time deduced from each resonance's linewidth will be also presented., Comment: 10 pages, 8 figures, to be published to J. Phys. Soc. Jpn Vol.72 No.1 (accepted)

Magnetooptical measurements of a quasi-two-dimensional (q2D) organic conductor (BEDT-TTF)2Br(DIA) (DIA=diiodoacetylene) were performed using a cavity perturbation technique with a millimeter vector network analyzer (MVNA). Harmonic resonances were observed periodically as a function of the inverse field up to the 7th order. This is the first observation of higher-order harmonics up to the 7th order in an organic conductor. The observed resonance is assigned as a periodic orbit resonance (POR) which arises from a q2D elliptic Fermi surface (FS). The obtained effective mass (4.7me) is consistent with Shubnikov-de Haas measurements. Temperature dependence of the spectra observed in two different sample configurations will be presented., Comment: 7 pages, 5 figures, to be published in J. Phys. Soc. Jpn Vol. 71 No.4