Searching for topological insulators in solids is one of the main issues of modern condensed matter physics since robust gapless edge or surface states of the topological insulators can be used as building blocks of next-generation devices. Enhancing spin-orbit couplings is a promising way to realize topological insulators in solids, whereas the amplitude of the spin-orbit couplings is not sufficiently large in most materials. Here we show a way to realize a topological state characterized by the quantized Zak phase, termed the Zak insulator, with spin-polarized edges in organic antiferromagnetic Mott insulators without relying on the spin-orbit coupling. The obtained Zak insulator can have a large charge gap compared to the conventional topological insulators, since Coulomb interactions mainly govern the amplitude of the charge gap in the antiferromagnetic Mott insulators. Besides the mean-field analysis, we demonstrate that the Zak insulator survives against electron correlation effects by calculating the many-body Zak phase. Our finding provides an unprecedented way to realize a topological state in strongly correlated electron systems.
Spin current--a flow of electron spins without a charge current--is an ideal information carrier free from Joule heating for electronic devices. The celebrated spin Hall effect, which arises from the relativistic spin-orbit coupling, enables us to generate and detect spin currents in inorganic materials and semiconductors, taking advantage of their constituent heavy atoms. In contrast, organic materials consisting of molecules with light elements have been believed to be unsuited for spin current generation. Here we show that a class of organic antiferromagnets with checker-plate type molecula…
Using Raman scattering, the quasi-two dimensional organic superconductor k-(BEDT-TTF)2Cu[N(CN)2]Br (T_c=11.8 K) and the related antiferromagnet k-(BEDT-TTF)2Cu[N(CN)2]Cl are studied. Raman scattering provides unique spectroscopic information about magnetic degrees of freedom that has been otherwise unavailable on such organic conductors. Below T=200 K a broad band at about 500 cm-1 develops in both compounds. We identify this band with two-magnon excitation. The position and the temperature dependence of the spectral weight are similar in the antiferromagnet and in the metallic Fermi-liquid. W…
The interdependence of antiferromagnetism and superconductivity in the Bechgaard salts series of organic conductors is examined in the light of the anomalous temperature dependence of the nuclear spin-lattice relaxation rate. We apply the renormalization group approach to the electron gas model to show that the crossover from antiferromagnetism to superconductivity along with the anomalous nuclear relaxation rate of the Bechgaard salts can be well described within a unified microscopic framework. For sizable nesting deviations of the Fermi surface, scaling theory reveals how pairing correlatio…
I apply a two-step renormalization group method to the study of the competition between antiferromagnetism (AFM) and superconductivity in an anisotropic 2D Hubbard model. I show that this simple model captures the essentials of the ground-state phases of the quasi 1D organic conductors. As found experimentally, the ground-state phase diagram is mostly AFM. The AFM is localized in the strong-coupling limit where the electrons are confined in the chains. It is an SDW in the weak-coupling limit where interchain hopping is present. There is a tiny region in the weak-coupling regime where transvers…
Superconductivity in the Bechgaard salts series of quasi-one-dimensional organic conductors occurs on the verge of spin-density-wave ordering when hydrostatic pressure is applied. The sequence of instabilities is intimately connected to normal state anomalies in various quantities like the temperature dependence of electrical transport and nuclear spin-lattice relaxation rate. We discuss how such a connection takes its origin in the interference between the different pairing mechanisms responsible for antiferromagnetism and superconductivity, a duo that can be comprehended in terms of a weak c…
Although the isotope effect in superconducting materials is well-documented, changes in the magnetic properties of antiferromagnets due to isotopic substitution are seldom discussed and remain poorly understood. This is perhaps surprising given the possible link between the quasi-two-dimensional (Q2D) antiferromagnetic and superconducting phases of the layered cuprates. Here we report the experimental observation of shifts in the Néel temperature and critical magnetic fields ($ΔT_{\rm N}/T_{\rm N}\approx 4%$; $ΔB_{\rm c}/B_{\rm c}\approx 4%$) in a Q2D organic molecular antiferromagnets on subs…
For temperatures T well above the ordering temperature T*=3.0+-0.2K the magnetic properties of the metal-organic material Mn[C10H6(OH)(COO)]2x2H20 built from Mn^2+ ions and 3-hydroxy-2-naphthoic anions can be described by a S=5/2 quantum antiferromagnet on a distorted honeycomb lattice with two different nearest neighbor exchange couplings J2 \approx 2J1 \approx 1.8K. Measurements of the magnetization M(H,T) as a function of a uniform external field H and of the uniform zero field susceptibility χ(T) are explained within the framework of a modified spin-wave approach which takes into account t…
The low-temperature electronic state of the layered organic charge-transfer salt $κ$-(BETS)$_2$FeCl$_4$ was probed by interlayer electrical resistance measurements under magnetic field. Both above and below $T_{\mathrm{N}}=0.47\,$K, the temperature of antiferromagnetic ordering of $3d$-electron spins of Fe$^{3+}$ localized in the insulating anion layers, a non-saturating linear $R(T)$ dependence has been observed. A weak superconducting signal has been detected in the antiferromagnetic state, at temperatures $\leq 0.2\,$K. Despite the very high crystal quality, only a tiny fraction of the samp…
A Hubbard model at half-filling on an anisotropic triangular lattice has been proposed as the minimal model to describe conducting layers of $κ-(BEDT-TTF)_2X$ organic materials. The model interpolates between the square lattice and decoupled chains. The $κ-(BEDT-TTF)_2X$ materials present many similarities with cuprates, such as the presence of unconventional metallic properties and the close proximity of superconducting and antiferromagnetic phases. As in the cuprates, spin fluctuations are expected to play a crucial role in the onset of superconductivity. We perform a weak-coupling renormali…
The band structure and magnetic properties of organic charge-transfer salt $λ$-(BEDSe-TTF)$_2$GaCl$_4$ (BEDSe-TTF: bis(ethylenediseleno)tetrathiafulvalene; abbreviated as $λ$-BEDSe) are investigated. The reported crystal structure is confirmed using X-ray diffraction measurements, and the transfer integrals are calculated. The degree of electron correlation $U/W$ ($U$: on-site Coulomb repulsion, $W$: bandwidth) of $λ$-BEDSe is larger than one and comparable to that of the isostructural Mott insulator $λ$-(ET)$_2$GaCl$_4$ (ET: bis(ethylenedithio)tetrathiafulvalene, abbreviated as $λ$-ET), where…
We give a quantitative analysis of the previously published nuclear magnetic resonance (NMR) experiments in the k-(ET)2X family of organic charge transfer salts by using the phenomenological spin fluctuation model of Moriya, and Millis, Monien and Pines (M-MMP). For temperatures above T_nmr ~ 50 K, the model gives a good quantitative description of the data in the metallic phases of several k-(ET)2X materials. These materials display antiferromagnetic correlation lengths which increase with decreasing temperature and grow to several lattice constants by T_nmr. It is shown that the fact that th…
We give a quantitative analysis of the published results of nuclear magnetic resonance (NMR) experiments for k-(ET)2X family of organic charge transfer salts by using the phenomenological spin fluctuation model of Moriya, and Millis, Monien and Pines (M-MMP). For temperatures above T_NMR ~ 50 K, the model gives a good quantitative description of the data for the paramagnetic metallic phase of several k-(ET)2X materials, with an antiferromagnetic correlation length which increases with decreasing temperature; growing to several lattice constants by T_NMR. It is shown that the fact that the dime…
We theoretically propose a mechanism for the anomalous Hall effect (AHE) in an antiferrromagnetic (AFM) state of $κ$-type organic conductors. We incorporate the spin-orbit coupling in the effective Hubbard model on the $κ$-type lattice structure taking into account the orientation of the molecules and their arrangement with dimerization. Treating this model by means of the Hartree-Fock approximation and the linear response theory, we find that an intrinsic contribution to the Hall conductivity becomes nonzero in the electron-doped AFM metallic phase with a small canted ferromagnetic moment. We…
Topological properties of physical systems are attracting tremendous interest. Recently, magnetic solid state compounds with and without magnetic order have become a focus. We show that ${\text{BiCu}}_{2}{\text{PO}}_{6}$ is the first gapful quantum antiferromagnet with a finite Zak phase, which characterises one-dimensional systems, and only the second with topological non-trivial triplon excitations. Surprisingly, in spite of the bulk-boundary correspondence no localised edge mode occurs. This unexpected behaviour is explained by the distinction between direct and indirect gaps among the trip…
We report the magnetic diffraction pattern and spin wave excitations in (CD$_3$)$_2$ND$_2$[Mn(DCO$_2$)$_3$] measured using elastic and inelastic neutron scattering. The magnetic structure is shown to be a G-type antiferromagnet with moments pointing along the $b$ axis. By comparison with simulations based on linear spin wave theory, we have developed a model for the magnetic interactions in this multiferroic metal-organic framework material. The interactions form a three-dimensional network with antiferromagnetic nearest-neighbour interactions along three directions of $J_1=-0.103(8)$~meV, $J_…
Magnetic properties of metal-organic coordination networks based on 3d transition metal atoms
Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；Paul Scherrer Institute（保罗谢尔研究所）；IKERBASQUE, Basque Foundation for Science（伊克尔巴斯基克科学基金会）；Tomsk State University（托木斯克州立大学）；Saint Petersburg State University（圣彼得堡国立大学）
In this article, I study magnetic response of electron wavefunctions in a commensurate collinear antiferromagnet. I show that, at a special set of momenta, hidden anti-unitary symmetry protects Kramers degeneracy of Bloch eigenstates against a magnetic field, pointing transversely to staggered magnetization. Hence a substantial momentum dependence of the transverse g-factor in the Zeeman term, turning the latter into a spin-orbit coupling, that may be present in materials from chromium to borocarbides, cuprates, pnictides, as well as organic and heavy fermion conductors.
Low Energy Excitations in a [4]Triangulene Honeycomb Antiferromagnet
University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Kavli Energy NanoScience Institute at the University of California Berkeley and the Lawrence Berkeley National Laboratory（加州大学伯克利分校与劳伦斯伯克利国家实验室卡弗里能源纳米科学研究所）
We construct a tight-binding model of [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ from Wannier orbital overlaps. Including interactions within the Jahn-Teller distorted Cu-centered $e_g$ Wannier orbitals leads to an effective Heisenberg model. The hyper-honeycomb lattice contains two symmetry distinct sublattices of Cu atoms arranged in coupled chains. One sublattice is strongly dimerized, the other forms isotropic antiferromagnetic chains. Integrating out the strongest (intradimer) exchange interactions leaves extremely weakly coupled Heisenberg chains, consistent with the observed low tem…
Submillimeter and millimeter wave electron spin resonance (ESR) measurements of the pi-d correlated organic conductor lambda-(BETS)2Fe0.6Ga0.4Cl4 have been performed. Antiferromagnetic resonance (AFMR) has been observed in the insulating antiferromagnetic phase, and its frequency-field dependence can be reproduced by the biaxial anisotropic AFMR theory. We find that in this alloy system, the easy-axis is near the b-axis, unlike previous results for the pure lambda-(BETS)2FeCl4 salts where it is closer to the c*-axis. We have also observed electron paramagnetic resonance (EPR) in the metallic p…
The electrical resistivity of the quasi-1D organic superconductor (TMTSF)2PF6 was recently measured at low temperature from the critical pressure needed to suppress the spin-density-wave state up to a pressure where superconductivity has almost disappeared. This data revealed a direct correlation between the onset of superconductivity at Tc and the strength of a non-Fermi-liquid linear term in the normal-state resistivity, going as r(T) = r0 + AT + BT2 at low temperature, so that A goes to 0 as Tc goes to 0. Here we show that the contribution of low-frequency antiferromagnetic fluctuations to …
Organic charge transfer salts show a variety of complex phases ranging from antiferromagnetic long-range order, spin liquid, bad metal or even superconductivity. A powerful method to investigate magnetism is spin-polarized inelastic neutron scattering. However, such measurements have often been hindered in the past by the small size of available crystals as well as by the fact that the spin in these materials is distributed over molecular rather than atomic orbitals and good estimates for the magnetic form factors are missing. By considering Wannier functions obtained from density functional t…
The occurrence of antiferromagnetism in kappa-(ET)_2X can be understood within an effective 1/2-filled band with dimers of ET molecules containing one hole each. We argue that while this effective model can describe the presence of antiferromagnetism, a complete description for these materials requires the correct carrier density of one-half per molecule. For dimerized and strongly frustrated 1/4-filled lattices we show that a singlet-paired state coexisting with charge ordering occurs that we have termed the Paired Electron Crystal (PEC). Here we investigate the 1/4-filled model on a dimerize…
Multiferroics, showing simultaneous ordering of electrical and magnetic degrees of freedom, are remarkable materials as seen from both the academic and technological points of view. A prominent mechanism of multiferroicity is the spin-driven ferroelectricity, often found in frustrated antiferromagnets with helical spin order. There, similar to conventional ferroelectrics, the electrical dipoles arise from an off-centre displacement of ions. However, recently a different mechanism, namely purely electronic ferroelectricity, where charge order breaks inversion symmetry, has attracted considerabl…
Magnetic structures of organic Mott insulators X[Pd(dmit)2]2 (X=Me4P, Me4Sb), of which electronic states are located near quantum spin liquid (X=EtMe3Sb), are demonstrated by 13C NMR. Antiferromagnetic spectra and nuclear relaxations show two distinct magnetic moments within each Pd(dmit)2 molecule, which cannot be described by single band dimer-Mott model and requires intramolecular electronic correlation. This unconventional fragmentation of S = 1/2 electron spin with strong quantum fluctuation is presumably caused by nearly degenerated intramolecular multiple orbitals, and shares a notion o…
I show that for a κ-type organic (BEDT-TTF)_2-X molecular crystal, a superconducting state with T_c ~ 10 K and gap nodes on the Fermi surface can be caused by short-ranged antiferromagnetic spin fluctuations. Using a two-band description for the anti-bonding orbitals on a BEDT-TTF dimer of the κ-type salt, and an intermediate local Coulomb repulsion between two holes on one dimer, the magnetic interaction and the superconducting gap-function are determined self consistently within the fluctuation exchange approximation. The pairing interaction is predominantly caused by inter-band coupling and…
We investigated the magnetism under a magnetic field in the quasi-two-dimensional organic Mott insulator $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl through magnetization and $^{13}$C-NMR measurements. We found that in the nominally paramagnetic phase (i.e., above Néel temperature) the field-induced local moments have a staggered component perpendicular to the applied field. As a result, the antiferromagnetic transition well defined at a zero field becomes crossover under a finite field. This unconventional behavior is qualitatively reproduced by the molecular-field calculation for Hamiltonian inclu…
We have measured the magnetization of the organic compound BIP-BNO (3,5'-bis(N-tert-butylaminoxyl)-3',5-dibromobiphenyl) up to 76 T where the magnetization is saturated. The S = 1/2 antiferromagnetic Heisenberg two-leg spin-ladder model accounts for the obtained experimental data regarding the magnetization curve, which is clarified using the quantum Monte Carlo method. The exchange constants on the rung and the side rail of the ladder are estimated to be J(rung)/kB = 65.7 K and J(leg)/kB = 14.1 K, respectively, deeply in the strong coupling region: J(rung)/J(leg) > 1.
We investigate by electrical transport the field-induced superconducting state (FISC) in the organic conductor $λ$-(BETS)$_2$FeCl$_4$. Below 4 K, antiferromagnetic-insulator, metallic, and eventually superconducting (FISC) ground states are observed with increasing in-plane magnetic field. The FISC state survives between 18 and 41 T, and can be interpreted in terms of the Jaccarino-Peter effect, where the external magnetic field {\em compensates} the exchange field of aligned Fe$^{3+}$ ions. We further argue that the Fe$^{3+}$ moments are essential to stabilize the resulting singlet, two-dimen…
Experimental quest for the hypothetical "quantum spin liquid" state has recently met a few promising candidate materials including organic salts κ-(ET)2Cu2(CN)3 and EtMe3Sb[Pd(dmit)2]2, S=1/2 triangular-lattice Heisenberg antiferromagnets consisting of molecular dimers. These compounds exhibit no magnetic ordering nor the spin freezing down to very low temperature, while various physical quantities exhibit gapless behaviors. Recent dielectric measurements revealed the glassy dielectric response suggesting the random freezing of the electric polarization degrees of freedom. Inspired by this obs…
$^{1}$H NMR and static susceptibility measurements have been performed in an organic Mott insulator with nearly isotropic triangular lattice, $κ$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$, which is a model system of frustrated quantum spins. The static susceptibility is described by the spin $S$ = 1/2 antiferromagnetic triangular-lattice Heisenberg model with the exchange constant $J$ $\sim$ 250 K. Regardless of the large magnetic interactions, the $^{1}$H NMR spectra show no indication of long-range magnetic ordering down to 32 mK, which is four-orders of magnitude smaller than $J$. These results su…
We solve the Sp(N) Heisenberg and SU(N) Hubbard-Heisenberg models on the anisotropic triangular lattice in the large-N limit. These two models may describe respectively the magnetic and electronic properties of the family of layered organic materials $κ$-(BEDT-TTF)$_2$X. The Heisenberg model is also relevant to the frustrated antiferromagnet, Cs$_2$CuCl$_4$. We find rich phase diagrams for each model. The Sp(N) antiferromagnet is shown to have five different phases as a function of the size of the spin and the degree of anisotropy of the triangular lattice. The effects of fluctuations at finit…
The $120^0$ ordered antiferromagnetic state of the Hubbard model on a triangular lattice presents an interesting case of $U$-controlled competing interactions and frustration. The spin stiffness is found to vanish at $U^* _{\rm stiff} \approx 6$ and the spin-wave energy $ω_M$ at ${\bf q}_M=(2π/3,0)$ etc. is found to vanish at $U_M ^* \approx 6.8$ due to competing spin couplings generated at finite $U$. The loss of magnetic order due to the magnetic instability at ${\bf q}_M$ yields a first-order quantum phase transition in the insulating state at $U=U_{\rm M}^*$. Implications of the quantum sp…
Muon spin relaxation measurements are reported on samples of dimethylammonium metal formates containing magnetic divalent nickel, cobalt, manganese, and copper ions. These hybrid organic-inorganic perovskites exhibit weak ferromagnetism and are, apart from the copper system, multiferroics with well separated magnetic and antiferroelectric transitions. We use muons to follow the sublattice magnetization, observing the effect of the spin reorientation transitions below TN and the criticality approaching TN. The multiferroic samples have three-dimensional antiferromagnetic interactions, but the c…
We posit that there exist deep and fundamental relationships between the above seemingly very different materials. The carrier concentration-dependences of the electronic behavior in the conducting organic charge-transfer solids and layered cobaltates are very similar. These dependences can be explained within a single theoretical model, - the extended Hubbard Hamiltonian with significant nearest neighbor Coulomb repulsion. Interestingly, superconductivity in the cobaltates seems to be restricted to bandfilling exactly or close to one-quarter, as in the organics. We show that dynamic Jahn-Tell…
In this article, I analyze the symmetries and degeneracies of electron eigenstates in a commensurate collinear antiferromagnet. In a magnetic field transverse to the staggered magnetization, a hidden anti-unitary symmetry protects double degeneracy of the Bloch eigenstates at a special set of momenta. In addition to this `Kramers degeneracy' subset, the manifold of momenta, labeling the doubly degenerate Bloch states in the Brillouin zone, may also contain an `accidental degeneracy' subset, that is not protected by symmetry and that may change its shape under perturbation. These degeneracies g…
We have investigated the charge ordering phase of the quasi one dimensional quantum antiferromagnet (TMTTF)$_2X$ ($X=$ SbF$_6$, AsF$_6$ and PF$_6$) using high fields/frequencies electron paramagnetic resonance. In addition to the uniform displacement of the counter anions involved in the charge order phase, we report the existence of a superlattice between the spin chains in the direction $c$, caused by the space modulation of the charge order. When the field is high enough, the magnetic decoupling of the spin chains allows us to estimate the interaction between the chains, $J_c<1$~mK, three o…
We study the influence of inelastic electron-electron scattering on the temperature variation of the Seebeck coefficient in the normal phase of quasi-one-dimensional organic superconductors. The theory is based on the numerical solution of the semi-classical Boltzmann equation for which the collision integral equation is solved with the aid of the electronic umklapp scattering vertex calculated by the renormalization group method. We show that the one-loop renormalization group flow of momentum and temperature dependent umklapp scattering, in the presence of nesting alterations of the Fermi su…
In the organic charge transfer salt k-(BETS)2Mn[N(CN)2]3 the metallic conductivity is provided by itinerant pi-electrons in the layers of BETS molecules, whereas magnetization is largely dominated by the localized d-electrons of the Mn2+ ions in the insulating anionic layers. We study magnetic properties of the compound in its low-temperature, Mott-insulating state by means of magnetic torque technique. The complex behavior of the torque can be qualitatively explained by the coexistence of two weakly interacting magnetic subsystems associated with paramagnetic d-electron spins and antiferromag…
A few organic conductors show a diversity of exciting properties like Mott insulating behaviour, spin liquid, antiferromagnetism, bad metal or unconventional superconductivity controlled by small changes in temperature, pressure or chemical substitution. While such a behaviour can be technologically relevant for functional switches, a full understanding of its microscopic origin is still lacking and poses a challenge in condensed matter physics since these phases may be a manifestation of electronic correlation. Here we determine from first principles the microscopic nature of the electronic p…
Organic solids host various electronic phases. Especially, a milestone compound of organic solid, $β'$-$X$[Pd(dmit)$_2$]$_2$ with $X$=EtMe$_3$Sb shows quantum spin-liquid (QSL) properties suggesting a novel state of matter. However, nature of the QSL has been largely unknown. Here, we computationally study five compounds comprehensively with different $X$ using 2D $ab$ $initio$ Hamiltonians and correctly reproduce experimental phase diagram with antiferromagnetic order for $X$=Me$_4$P, Me$_4$As, Me$_4$Sb, Et$_2$Me$_2$As and a QSL for $X$=EtMe$_3$Sb without adjustable parameters. We find that t…
The layered organic compounds, kappa-(BEDT-TTF)_2Cu[N(CN)_2X (X=Cl, Br) are metals at ambient temperatures. At low temperatures, the Cl compound is a weakly ferromagnetic Mott insulator while the isostructural Br compound is a superconductor. We find by conduction electron spin resonance (CESR) and antiferromagnetic resonance (AFMR) an extreme anisotropy of spin transport and magnetic interactions in these materials. In the metallic state spin diffusion is confined to single molecular layers within the spin lifetime of 10^-9 s. Electrons diffuse several hundreds of nm without hopping to the ne…
In the quest for materials with unconventional quantum phases, the organic triangular-lattice antiferromagnet $κ$-(ET)$_2$Cu$_2$(CN)$_3$ has been extensively discussed as a quantum spin liquid (QSL) candidate. Recently, an intriguing quantum critical behaviour was suggested from low-temperature magnetic torque experiments. Through microscopic analysis of all anisotropic contributions, including Dzyaloshinskii-Moriya and multi-spin scalar chiral interactions, we highlight significant deviations of the experimental observations from a quantum critical scenario. Instead, we show that disorder-ind…
We present the results of first-principle calculations using the Vienna Ab-initio Simulation Package (VASP) for a new class of organometallics labeled TM3C6O6 (TM =Sc, Ti, V, Cr, Fe, Co, Ni and Cu) in the form of planar, two-dimensional, periodic free-standing layers. These materials, which can be produced by on-surface coordination on metallic surfaces, have a kagome lattice of TM ions. Calculating the structural properties, we show that all considered materials have local magnetic moments in the ground state, but four of them (with Fe, Co, Ni and Cu) show spin-crossover behavior by changing …
We study spin fluctuation (SF) mediated superconductivity (SC) in a half-filled square lattice Hubbard model with the transfer matrices -t between nearest neighbor sites and -t' between a half of next nearest neighbor sites neighboring along only one of the <1,1> directions, considering application of this model to organic kappa-(BEDT-TTF)2X compounds. Varying the t'/t value from 0 to 1, one can interpolate between a square and an equilateral triangular lattice, the latter giving frustration to antiferromagnetically (AF) coupled spin systems. Within the fluctuation exchange (FLEX) approximatio…
$^{77}$Se-NMR spectrum and frequency shift measurements in the paramagnetic metal (PM) and antiferromagnetic insulating (AFI) phases are reported for a small single crystal of the organic conductor $λ-$(BETS)$_{2}$FeCl$_{4}$ as a function of temperature ($T$) and field alignment for an applied magnetic field $B_{0}$ = 9 T. The results show that in the low $T$ limit, where the localized Fe$^{3+}$ spins ($S_{d}$ = 5/2) are almost fully polarized, the conduction electrons (Se $π$-electrons, spin $s_π$ = 1/2) in the BETS molecules experience an exchange field ($\bf{B}$$_{πd}$) from the Fe$^{3+}$ s…
The two-dimensional organic conductor lambda-(BETS)2FeCl4 has an unusual phase diagram as a function of temperature and magnetic field that includes a paramagnetic metal (PM) phase, an antiferromagnetic insulating (AFI) phase, and a field-induced superconducting phase [S. Uji, H. Kobayashi, L. Balicas, and James S. Brooks, Adv. Mater. 14, 243 (2002), and cited references]. Here, we report a preliminary investigation of the PM and AFI phases at 9.0 T over the temperature range 2.0-180 K that uses proton NMR measurements of the spectrum, the spin-lattice relaxation rate (1/T1), and the spin echo…
The square-lattice quantum Heisenberg antiferromagnet displays a pronounced anomaly of unknown origin in its magnetic excitation spectrum. The anomaly manifests itself only for short wavelength excitations propagating along the direction connecting nearest neighbors. Using polarized neutron spectroscopy, we have fully characterized the magnetic fluctuations in the model metal-organic compound CFTD, revealing an isotropic continuum at the anomaly indicative of fractional excitations. A theoretical framework based on the Gutzwiller projection method is developed to explain the origin of the cont…
The ground state of an S=1/2 antiferromagnetic Heisenberg model on a spatially anisotropic triangular lattice, which is an effective model of Mott insulators on a triangular layer of organic charge transfer salts or Cs2CuCl4, is numerically studied. We apply a numerical variational method by using a tensor network with entanglement renormalization, which improves the capability of describing a quantum state. Magnetic ground states are identified for 0.7 <= J2/J1 <= 1 in the thermodynamic limit, where J1 and J2 denote the inner-chain and inter-chain coupling constants, respectively. Except for …
At zero temperature and strong applied magnetic fields the ground sate of an anisotropic antiferromagnet is a saturated paramagnet with fully aligned spins. We study the quantum phase transition as the field is reduced below an upper critical $H_{c2}$ and the system enters a XY-antiferromagnetic phase. Using a bond operator representation we consider a model spin-1 Heisenberg antiferromagnetic with single-ion anisotropy in hyper-cubic lattices under strong magnetic fields. We show that the transition at $H_{c2}$ can be interpreted as a Bose-Einstein condensation (BEC) of magnons. The theoretic…
We present the results of $^{69,71}$Ga-NMR measurements on an organic antiferromagnet $λ$-(BEDSe-TTF)$_2$GaCl$_4$ [BEDSe-TTF=bis(ethylenediseleno)tetrathiafulvalene], with comparison to reports on $λ$-(BETS)$_2$GaCl$_4$ [BETS=bis(ethylenedithio)tetraselenafulvalene] [T. Kobayashi et al., Phys. Rev. B 102, 235131 (2020)]. We found that the dynamics of two crystallographically independent ethylene groups induce two types of quadrupolar relaxation in the high-temperature region. As the ethylene motion freezes, hyperfine (HF) interactions develop between $π$ spin and Ga nuclear spin below 100 K, a…
We explore the effect of the third nearest-neighbors on the magnetic properties of the Heisenberg model on an anisotropic triangular lattice. We obtain the phase diagram of the model using Schwinger-boson mean-field theory. Competition between Néel, spiral and collinear magnetically ordered phases is found as we vary the on the ratios of the nearest, J1, next-nearest, J2, and third-nearest, J_3, neighbor exchange couplings. A spin liquid phase is stabilized between the spiral and collinear ordered states when J2/J1 < 1.8 for rather small J3/J1 < 0.1. The lowest energy two-spinon dispersions re…
Most of solid-state spin physics arising from spin-orbit coupling, from fundamental phenomena to industrial applications, relies on symmetry-protected degeneracies. So does the Zeeman spin-orbit coupling, expected to manifest itself in a wide range of antiferromagnetic conductors. Yet, experimental proof of this phenomenon has been lacking. Here, we demonstrate that the Néel state of the layered organic superconductor $κ$-(BETS)$_2$FeBr$_4$ shows no spin modulation of the Shubnikov-de Haas oscillations, contrary to its paramagnetic state. This is unambiguous evidence for the spin degeneracy of…
We review recent progress in understanding the different spatial broken symmetries that occur in the normal states of the family of charge-transfer solids (CTS) that exhibit superconductivity (SC), and discuss how this knowledge gives insight to the mechanism of the unconventional SC in these systems. We show that a unified theory of the diverse broken symmetry states necessarily requires explicit incorporation of strong electron-electron interactions and lattice discreteness, and most importantly, the correct bandfilling of one-quarter. Uniquely in the quarter-filled band, there is a very str…
