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External pressure and associated changes in lattice structures are key to realizing exotic quantum phases such as high-$T_{\rm c}$ superconductivity. While applying external pressure is a standard method to induce novel lattice structures, its impact on organic molecular crystals has been less explored. Here we report a unique structural phase transition in (DMET-TTF)$_2$AuBr$_2$ under pressure. By combining advanced high-pressure techniques and $ab$ $initio$ calculations, we elucidate that (DMET-TTF)$_2$AuBr$_2$ undergoes a transition from a quasi-one-dimensional lattice to a nearly perfect rectangular lattice at 0.9 GPa. This transition leads to the realization of an antiferromagnetic Mott insulator with $T_{\rm N}=66$ K, the highest $T_{\rm N}$ in low-dimensional molecular crystal solids to date. Upon increasing the pressure, the antiferromagnetic ordering is suppressed, and a superconducting phase with $T_{\rm c}=4.8$ K emerges around 6 GPa. Our study reveals the significant impact of external pressure on lattice structures of organic molecular crystals and highlights the intricate relationship between geometrical frustration and superconductivity. Our findings also pave the way for realizing functional organic molecular crystals through changes in lattice structures by pressure., Comment: 11 pages, 7 figures, 3 Tables

Spin current, a key concept in spintronics that carries spin angular momentum, has a non-unique definition due to the non-conservation of spins in solids. While two primary definitions exist -- conventional spin current and conserved spin current -- their validity has not been quantitatively examined. Here, we examine the validity of these definitions of spin current by comparing their spin Hall conductivities to the spin accumulation on edges of materials calculated in a real-time evolution simulation. Employing the Kane-Mele model with the Rashba term, which explicitly violates spin conservation, we reveal that the spin Hall conductivities calculated under both definitions fail to reproduce the simulated results of spin accumulation when the Rashba term is large. Our results suggest that the standard definitions of spin current and the associated spin Hall conductivity do not give an accurate quantitative estimate of spin accumulation. This conclusion indicates that real-time simulations are necessary to accurately estimate spin accumulation on edges/surfaces of materials., Comment: 5 pages, 3 figures

We present a combined experimental and theoretical study on the quasi-one-dimensional organic conductor (TMTTF)$_2$PF$_6$, and elucidate the variation of its physical properties under pressure. We fully resolve the crystal structure by single crystal x-ray diffraction measurements using a diamond anvil cell up to 8 GPa, and based on the structural data, we perform first-principles density-functional theory calculations and derive the $ab$ $initio$ extended Hubbard-type Hamiltonians. Furthermore, we compare the behavior of the resistivity measured up to 3 GPa using a BeCu clamp-type cell and the ground state properties of the obtained model numerically calculated by the many-variable variational Monte Carlo method. Our main findings are as follows: i) The crystal was rapidly compressed up to about 3 GPa where the volume drops to 80% and gradually varies down to 70% at 8 GPa. The transfer integrals increase following such behavior whereas the screened Coulomb interactions decrease, resulting in a drastic reduction of correlation effect. ii) The degree of dimerization in the intrachain transfer integrals, as the result of the decrease in structural dimerization together with the change in the intermolecular configuration, almost disappears above 4 GPa; the interchain transfer integrals also show characteristic variations under pressure. iii) The results of identifying the characteristic temperatures in the resistivity and the charge and spin orderings in the calculations show an overall agreement: The charge ordering sensitively becomes unstable above 1 GPa, while the spin ordering survives up to higher pressures. These results shed light on the similarities and differences between applying external pressure and substituting the chemical species (chemical pressure)., Comment: 13 pages, 10 figures

Quantum entanglement in strongly correlated electron systems often leads to exotic elementary excitations. Quantum spin liquids (QSLs) provide a paradigmatic example, where the elementary excitations are described by fractional quasiparticles such as spinons. However, such fractional quasiparticles behave differently from electrons, making their experimental identification challenging. Here, we theoretically investigate the spin Seebeck effect, which is a thermoelectric response via a spin current, as an efficient probe of the fractional quasiparticles in QSLs, focusing on the Kitaev honeycomb model. By comprehensive studies using the real-time dynamics, the perturbation theory, and the linear spin-wave theory based on the tunnel spin-current theory, we find that the spin current is induced by thermal gradient in the Kitaev spin liquid, via the low-energy fractional Majorana excitations. This underscores the ability of Majorana fermions to carry spin current, despite lacking spin angular momentum. Furthermore, we find that the induced spin current changes its sign depending on the sign of the Kitaev interaction, indicating that the Majorana fermions contribute to the spin current with (up-)down-spin like nature when the exchange coupling is (anti)ferromagnetic. Thus, in contrast to the negative spin current already found in a one-dimensional QSL, our finding reveals that the spin Seebeck effect can exhibit either positive or negative signals, contingent upon the nature of fractional excitations in the QSLs. We also clarify contrasting field-angle dependence between the Kitaev spin liquid in the low-field limit and the high-field ferromagnetic state, which is useful for the experimental identification. Our finding suggests that the spin Seebeck effect could be used not only to detect fractional quasiparticles emerging in QSLs but also to generate and control them., Comment: 16 pages, 10 figures

The study of the magnetic order has recently been invigorated by the discovery of exotic collinear antiferromagnets with time-reversal symmetry breaking. Examples include altermagnetism and compensated ferrimagnets, which show spin splittings of the electronic band structures even at zero net magnetization, leading to several unique transport phenomena, notably spin-current generation. Altermagnets demonstrate anisotropic spin splitting, such as $d$-wave, in momentum space, whereas compensated ferrimagnets exhibit isotropic spin splitting. However, methods to realize compensated ferrimagnets are limited. Here, we demonstrate a method to realize a fully compensated ferrimagnet with isotropic spin splitting utilizing the dimer structures inherent in organic compounds. Moreover, based on $ab$ $initio$ calculations, we find that this ferrimagnet can be realized in the recently discovered organic compound (EDO-TTF-I)$_2$ClO$_4$. Our findings provide an unprecedented strategy for using the dimer degrees of freedom in organic compounds to realize fully compensated ferrimagnets with colossal spin splitting., Comment: 15 pages, 10 figures

Frustrated magnets with degenerate ground states exhibit exotic ground states and rich phase structures when perturbations and/or thermal fluctuations lift the degeneracy. In two-dimensional models with short-range interactions, continuous symmetries cannot spontaneously break at finite temperatures, leading to the suppression of conventional magnetic long-range ordering (LRO). In this paper, we numerically study the classical $J_1$-$J_2$ $XY$ antiferromagnet on the kagome lattice as a prototype model of such frustrated magnets, where $J_2$ denotes the next-nearest-neighbor exchange interaction. We map out the $J_2$-$T$ phase diagram of this model employing extensive classical Monte Carlo (MC) simulations. The obtained phase diagram features Berezinskii-Kosterlitz-Thouless (BKT) transitions of $q=0$, $\sqrt{3}\times\sqrt{3}$ magnetic orders, and octupole orders, in addition to finite-temperature phase transitions of both ferrochiral and antiferrochiral long-range orders. Additionally, we find a non-trivial first-order transition for antiferromagnetic $J_2/J_1 < 0$. The origin of this transition is discussed in the context of non-local loop structures present in local $120^\circ$ spin structures.

The realization of topological insulators induced by correlation effects is one of the main issues of modern condensed matter physics. An intriguing example of the correlated topological insulators is a magnetic Chern insulator induced by a noncoplanar multiple-Q magnetic order. Although the realization of the magnetic Chern insulator has been studied in the classical limit of the Kondo lattice model, research on the magnetic Chern insulator in the original Kondo lattice model is limited. Here, we investigate the possibility of the many-body Chern insulator with the noncoplanar triple-Q magnetic order in the Kondo lattice model on a triangular lattice. Using the many-variable variational Monte Carlo method, we reveal that the triple-Q magnetic order becomes a ground state at quarter filling in an intermediate Kondo coupling region. We also show that the many-body Chern number is quantized to one in the triple-Q magnetic ordered phase utilizing the polarization operators. Our results provide a pathway for the realization of the many-body Chern insulator in correlated electron systems., Comment: 7 pages, 5 figures

H-wave is an open-source software package for performing the Hartree--Fock approximation (HFA) and random phase approximation (RPA) for a wide range of Hamiltonians of interacting fermionic systems. In HFA calculations, H-wave examines the stability of several symmetry-broken phases, such as anti-ferromagnetic and charge-ordered phases, in the given Hamiltonians at zero and finite temperatures. Furthermore, H-wave calculates the dynamical susceptibilities using RPA to examine the instability toward the symmetry-broken phases. By preparing a simple input file for specifying the Hamiltonians, users can perform HFA and RPA for standard Hamiltonians in condensed matter physics, such as the Hubbard model and its extensions. Additionally, users can use a Wannier90-like format to specify fermionic Hamiltonians. A Wannier90 format is implemented in RESPACK to derive ab initio Hamiltonians for solids. HFA and RPA for the ab initio Hamiltonians can be easily performed using H-wave. In this paper, we first explain the basis of HFA and RPA, and the basic usage of H-wave, including download and installation. Thereafter, the input file formats implemented in H-wave, including the Wannier90-like format for specifying the interacting fermionic Hamiltonians, are discussed. Finally, we present several examples of H-wave such as zero-temperature HFA calculations for the extended Hubbard model on a square lattice, finite-temperature HFA calculations for the Hubbard model on a cubic lattice, and RPA in the extended Hubbard model on a square lattice., Comment: 15 pages, 7 figures

$\mathcal{H}\Phi$ [$aitch$-$phi$] is an open-source software package of numerically exact and stochastic calculations for a wide range of quantum many-body systems. In this paper, we present the newly added functions and the implemented methods in vers. 2 and 3. In ver. 2, we implement spectrum calculations by the shifted Krylov method, and low-energy excited state calculations by the locally optimal blocking preconditioned conjugate gradient (LOBPCG) method. In ver. 3, we implement the full diagonalization method using ScaLAPACK and GPGPU computing via MAGMA. We also implement a real-time evolution method and the canonical thermal pure quantum (cTPQ) state method for finite-temperature calculations. The Wannier90 format for specifying the Hamiltonians is also implemented. Using the Wannier90 format, it is possible to perform the calculations for the $ab$ $initio$ low-energy effective Hamiltonians of solids obtained by the open-source software RESPACK. We also update Standard mode $\unicode{x2014}$simplified input format in $\mathcal{H}\Phi$$\unicode{x2014}$ to use these functions and methods. We explain the basics of the implemented methods and how to use them., Comment: 21 pages, 10 figures, 2 tables

Dirac semi-metal with magnetic atoms as constituents delivers an interesting platform to investigate the interplay of Fermi surface (FS) topology, electron correlation, and magnetism. One such family of semi-metal is YbMn$Pn_2$ ($Pn$ = Sb, Bi), which is being actively studied due to the intertwined spin and charge degrees of freedom. In this Letter, we investigate the relationship between the magnetic/crystal structures and FS topology of YbMnSb$_2$ using single crystal x-ray diffraction, neutron scattering, magnetic susceptibility, magnetotransport measurement and complimentary DFT calculation. Contrary to previous reports, the x-ray and neutron diffraction reveal that YbMnSb$_2$ crystallizes in an orthorhombic $Pnma$ structure with notable anti-phase displacement of the magnetic Mn ions that increases in magnitude upon cooling. First principles DFT calculation reveals a reduced Brillouin zone and more anisotropic FS of YbMnSb$_2$ compared to YbMnBi$_2$ as a result of the orthorhombicity. Moreover, the hole type carrier density drops by two orders of magnitude as YbMnSb$_2$ orders antiferromagnetically indicating band folding in magnetic ordered state. In addition, the Landau level fan diagram yields a non-trivial nature of the SdH quantum oscillation frequency arising from the Dirac-like Fermi pocket. These results imply that YbMnSb$_2$ is an ideal platform to explore the interplay of subtle lattice distortion, magnetic order, and topological transport arising from relativistic quasiparticles., Comment: 11 pages, contains 4 figures and 7 Supplemental Figures

The Kitaev model offers a platform for quantum spin liquids (QSLs) with fractional excitations, itinerant Majorana fermions and localized fluxes. Since these fractional excitations could be utilized for quantum computing, how to create, observe, and control them through the spin degree of freedom is a central issue. Here, we study dynamical spin transport in a wide range of frequency for the Kitaev-Heisenberg model, by applying an AC magnetic field to an edge of the system. We find that, in the Kitaev QSL phase, spin polarizations at the other edge are resonantly induced in a specific spin component, even though the static spin correlations are vanishingly small. This interedge spin resonance appears around the input frequency over the broad frequency range. Comparing with the dynamical spin correlations, we clarify that the resonance is governed by the itinerant Majorana fermions with a broad continuum excitation spectrum, which can propagate over long distances, although it vanishes for the pure Kitaev model because of accidental degeneracy and requires weak Heisenberg interactions. We also find that the spin polarizations in the other spin components are weakly induced at an almost constant frequency close to the excitation gap of the localized fluxes, irrespective of the input frequency. These results demonstrate that the dynamical spin transport is a powerful probe of the fractional excitations in the Kitaev QSL. Possible experimental realization of the interedge spin resonance is discussed., Comment: 12 pages, 9 figure

We develop the interface tool $\verb|wan2respack|$, which connects $\verb|RESPACK|$ (software that derives the low-energy effective Hamiltonians of solids) with $\verb|Wannier90|$ (software that constructs Wannier functions). $\verb|wan2respack|$ converts the Wannier functions obtained by $\verb|Wannier90|$ into those used in $\verb|RESPACK|$, which is then used to derive the low-energy effective Hamiltonians of solids. In this paper, we explain the basic usage of $\verb|wan2respack|$ and show its application to standard compounds of correlated materials, namely, the correlated metal SrVO$_3$ and the high-$T_{c}$ superconductor La$_2$CuO$_4$. Furthermore, we compare the low-energy effective Hamiltonians of these compounds using Wannier functions obtained by $\verb|Wannier90|$ and those obtained by $\verb|RESPACK|$. We confirm that both types of Wannier functions give the same Hamiltonians. This benchmark comparison demonstrates that $\verb|wan2respack|$ correctly converts Wannier functions in the $\verb|Wannier90|$ format into those in the $\verb|RESPACK|$ format., Comment: 10 pages, 6 figures

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., Comment: 8 pages, 4 figures

An $ab$ $initio$ investigation of the family of molecular compounds TM$_2$$X$ is conducted, where TM is either TMTSF or TMTTF and $X$ takes centrosymmetric monovalent anions. By deriving the extended Hubbard-type Hamiltonians from first-principles band calculations and evaluating not only the intermolecular transfer integrals but also the Coulomb parameters, we discuss their material dependence in the unified phase diagram. Furthermore, we apply the many-variable variational Monte Carlo method to accurately determine the symmetry-breaking phase transitions, and show the development of the charge and spin orderings. We show that the material-dependent parameter can be taken as the correlation effect, represented by the value of the screened on-site Coulomb interaction $U$ relative to the intrachain transfer integrals, for the comprehensive understanding of the spin and charge ordering in this system., Comment: 9 pages, 5 figures, and 2 tables

To determine how electron correlations open a gap in two-dimensional massless Dirac electrons in the organic compounds $\alpha$-(BEDT-TTF)$_2$I$_3$ [$\alpha$-(ET)$_2$I$_3$] and $\alpha$-(BEDT-TSeF)$_2$I$_3$ [$\alpha$-(BETS)$_2$I$_3$], we derive and analyze $ab$ $initio$ low-energy effective Hamiltonians for these two compounds. We find that the horizontal stripe charge ordering opens a gap in the massless Dirac electrons in $\alpha$-(ET)$_2$I$_3$, while an insulating phase without explicit symmetry breaking appears in $\alpha$-(BETS)$_2$I$_3$. We clarify that the combination of the anisotropic transfer integrals and the electron correlations induces a dimensional reduction in the spin correlations, i.e., one-dimensional spin correlations develop in $\alpha$-(BETS)$_2$I$_3$. We show that the one-dimensional spin correlations open a gap in the massless Dirac electrons. Our finding paves the way for opening gaps for massless Dirac electrons using strong electronic correlations., Comment: 9 pages, 2 tables, and 6 figures. The input and output files of the ab initio and the mVMC calculations are available at https://isspns-gitlab.issp.u-tokyo.ac.jp/k-yoshimi/alpha-salts

We propose silver-based oxides with layered perovskite structure as candidates of exhibiting intriguing feature of strongly correlated electrons. The compounds show unique covalence between Ag d and O p orbitals with the strong electron correlation of their antibonding orbital similar to the copper oxide high-temperature superconductors, but stronger covalency and slightly smaller correlation strength. We examine $A_2$AgO$_2X_2$ with $A$ =Sr and Ba and $X$ =F, I and Cl in detail. Among them, Sr$_2$AgO$_2$F$_2$ has the largest effective onsite Coulomb repulsion and shows an antiferromagnetic insulating ground state, which competes with correlated metals. It offers features both similar and distinct from the copper oxides, and paves a new route. The possibility of superconductivity in doped systems is discussed., Comment: 25 pages, 21 figures, and 17 tables

Organic solids host various electronic phases. Especially, a milestone compound of organic solid, $\beta'$-$X$[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 the QSL for $X$=EtMe$_3$Sb exhibits 1D nature characterized by algebraic decay of spin correlation along one direction, while exponential decay in the other direction, indicating dimensional reduction from 2D to 1D. The 1D nature indeed accounts for the experimental specific heat, thermal conductivity and magnetic susceptibility. The identified QSL, however, preserves 2D nature as well consistently with spin fractionalization into spinon with Dirac-like gapless excitations and reveals duality bridging the 1D and 2D QSLs., Comment: 12 pages, 8 figures, 2 tables

The molecular solids $\beta^\prime$-$X$[Pd(dmit)$_2$]$_2$ (where $X$ represents a cation) are typical compounds whose electronic structures are described by single-orbital Hubbard-type Hamiltonians with geometrical frustration. Using the $ab$ $initio$ downfolding method, we derive the low-energy effective Hamiltonians for $\beta^\prime$-$X$[Pd(dmit)$_2$]$_2$ with available room- and low-temperature structures. We find that the amplitudes of the Coulomb interactions and the anisotropy of the hopping parameters in the effective Hamiltonians are sensitive to the changes in the lattice constants induced by lowering the temperature. The obtained effective Hamiltonians are analyzed using the exact diagonalization method with the boundary-condition average. We find that a significant reduction of the antiferromagnetic ordered moment occurs in the effective Hamiltonian of $\beta^\prime$-EtMe$_3$Sb[Pd(dmit)$_2$]$_2$ with the low-temperature structure. The reduction is consistent with the quantum spin liquid behavior observed in experiments. The comprehensive derivations of the effective Hamiltonians and exact-diagonalization analyses of them will clarify the microscopic origins of the exotic quantum states of matter found in $\beta^\prime$-$X$[Pd(dmit)$_2$]$_2$ such as the quantum spin liquid behavior., Comment: 12 pages, 6 figures, 1 table

High-temperature superconductivity occurs in strongly correlated materials such as copper oxides and iron-based superconductors. Numerous experimental and theoretical works have been done to identify the key parameters that induce high-temperature superconductivity. However, the key parameters governing the high-temperature superconductivity remain still unclear, which hamper the prediction of superconducting critical temperatures ($T_\text{c}$s) of strongly correlated materials. Here by using data-science techniques, we clarified how the microscopic parameters in the $ab$ $initio$ effective Hamiltonians correlate with the experimental $T_\text{c}$s in iron-based superconductors. We showed that a combination of microscopic parameters can characterize the compound-dependence of $T_\text{c}$ using the principal component analysis. We also constructed a linear regression model that reproduces the experimental $T_\text{c}$ from the microscopic parameters. Based on the regression model, we showed a way for increasing $T_\text{c}$ by changing the lattice parameters. The developed methodology opens a new field of materials informatics for strongly correlated electron systems., Comment: 16 pages, 7 figures, 4 tables

We theoretically propose the long-range spin transport mediated by the gapless surface states of topological Dirac semimetal (TDSM). Low-dissipation spin current is a building block of next-generation spintronics devices. While conduction electrons in metals and spin waves in ferromagnetic insulators (FMIs) are the major carriers of spin current, their propagation length is inevitably limited due to the Joule heating or the Gilbert damping. In order to suppress dissipation and realize long-range spin transport, we here make use of the spin-helical surface states of TDSMs, such as $\mathrm{Cd_3 As_2}$ and $\mathrm{Na_3 Bi}$, which are robust against disorder. Based on a junction of two FMIs connected by a TDSM, we demonstrate that the magnetization dynamics in one FMI induces a spin current on the TDSM surface flowing to the other FMI. By both the analytical transport theory on the surface and the numerical simulation of real-time evolution in the bulk, we find that the induced spin current takes a universal semi-quantized value that is insensitive to the microscopic coupling structure between the FMI and the TDSM. We show that this surface spin current is robust against disorder over a long range, which indicates that the TDSM surface serves as a promising system for realizing spintronics devices., Comment: 16 pages, 11 figures

This study demonstrates that the zeros of the diagonal components of Green functions are key quantities that can detect non-interacting topological insulators. We show that zeros of the Green functions traverse the band gap in the topological phases. The traverses induce the crosses of zeros, and the zeros' surface in the band gap, analogous to the Fermi surface of metals. By calculating the zeros of the microscopic models, we show the traverses of the zeros universally appear in all six classes of conventional non-interacting topological insulators. By utilizing the eigenvector-eigenvalue identity, which is a recently rediscovered relation in linear algebra, we prove that the traverses of the zeros in the bulk Green functions are guaranteed by the band inversions, which occur in the topological phases. The relevance of the zeros to detecting the exotic topological insulators such as the higher-order topological insulators is also discussed. For the Hamiltonians with the nearest-neighbor hoppings, we also show that the gapless edge state guarantees the zeros' surfaces in the band gap. The analysis demonstrates that the zeros can be used to detect a wide range of topological insulators and thus useful for searching new topological materials., Comment: 21 pages, 1 table, 14 figures

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)$_{2}$]$_{2}$., Comment: 11 pages, 11 figures, 1 table

We develop K$\omega$, an open-source linear algebra library for the shifted Krylov subspace methods. The methods solve a set of shifted linear equations $(z_k I-H)x^{(k)}=b\, (k=0,1,2,...)$ for a given matrix $H$ and a vector $b$, simultaneously. The leading order of the operational cost is the same as that for a single equation. The shift invariance of the Krylov subspace is the mathematical foundation of the shifted Krylov subspace methods. Applications in materials science are presented to demonstrate the advantages of the algorithm over the standard Krylov subspace methods such as the Lanczos method. We introduce benchmark calculations of (i) an excited (optical) spectrum and (ii) intermediate eigenvalues by the contour integral on the complex plane. In combination with the quantum lattice solver $\mathcal{H} \Phi$, K$\omega$ can realize parallel computation of excitation spectra and intermediate eigenvalues for various quantum lattice models., Comment: 12 pages, 5 figures

RESPACK is a first-principles calculation software for evaluating the interaction parameters of materials and is able to calculate maximally localized Wannier functions, response functions based on the random phase approximation and related optical properties, and frequency-dependent electronic interaction parameters. RESPACK receives its input data from a band-calculation code using norm-conserving pseudopotentials with plane-wave basis sets. Automatic generation scripts that convert the band-structure results to the RESPACK inputs are prepared for xTAPP and Quantum ESPRESSO. An input file for specifying the RESPACK calculation conditions is designed pursuing simplicity and is given in the Fortran namelist format. RESPACK supports hybrid parallelization using OpenMP and MPI and can treat large systems including a few hundred atoms in the calculation cell., Comment: 22pages, 18 figures, 16 tables, RESPACK website: https://sites.google.com/view/kazuma7k6r

We theoretically manifest that the edge of a quantum spin Hall insulator (QSHI), attached to an insulating ferromagnet (FM), can realize a highly efficient spin-to-charge conversion. Based on a one-dimensional QSHI-FM junction, the electron dynamics on the QSHI edge is analyzed, driven by a magnetization dynamics in the FM. Under a large gap opening on the edge from the magnetic exchange coupling, we find that the spin injection into the QSHI edge gets suppressed while the charge current driven on the edge gets maximized, demanded by the band topology of the one-dimensional helical edge states., Comment: 11 pages, 4 figures, to be published in Phys. Rev. Research

We study the time-development processes of spin and charge transport phenomena in a topological Dirac semimetal attached to a ferromagnetic insulator with a precessing magnetization. Compared to conventional normal metals, topological Dirac semimetals manifest a large inverse spin Hall effect when a spin current is pumped from the attached ferromagnetic insulator. It is shown that the induced charge current is semi-quantized, i.e., it depends only on the distance between the two Dirac points in momentum space and hardly depends on the disorder strength when the system remains in the topological Dirac semimetal phase. As an inverse effect, we show that the electric field applied to the topological Dirac semimetal exerts a spin torque on the local magnetization in the ferromagnetic insulator via the exchange interaction and the semi-quantized spin Hall effect. Our study demonstrates that the topological Dirac semimetal offers a less-dissipative platform for spin-charge conversion and spin switching., Comment: 6 pages, 3 figures

Real-time evolution and charge pumping in magnetic Weyl semimetals are studied by solving the time-dependent Schr\"{o}dinger equations. In the adiabatic limit of the real-time evolution, we show that the total pumped charge is quantized in the magnetic Weyl semimetals as in the quantum Hall system although the Weyl semimetal has no bulk gap. We examine how the disorder affects the charge pumping. As a result, we show that the quantized pumped charge is robust against the small disorder and find that the pumped charge increases in the intermediate disorder region. We also examine the doping effects on the charge pumping and show that the remnant of the quantized pumped charge at zero doping can be detected. Our results show that the real-time evolution is a useful technique for detecting the topological properties of the systems with no bulk gap and/or disorders., Comment: 11 pages, 9 figures

We study frustrated spin-1/2 dimer systems in two dimensions with a bilayer structure, where spins are ferromagnetically coupled in dimers. Our model includes frustrated two-spin exchange interactions as well as four-spin interaction. We pay particular attention to the spin nematic phase, which does not exhibit any magnetic (spin-dipole) order but has a spin-quadrupolar long-range order. Employing a perturbation calculation, a mean-field approximation, and a numerical many-variable variational Monte Carlo method, we determine ground-state phase diagrams on various two-dimensional lattices. It is found that the model exhibits the spin nematic phase with ferro-quadrupolar order in a wide parameter region, in addition to conventional magnetically-ordered phases. In particular, it is shown that even when the four-spin interactions are absent, frustrated two-spin exchange interactions can realize the spin nematic phase as a result of strong interdimer correlations. It is also found that the phase transitions between the spin nematic phase and antiferromagnetic phases can be continuous. Furthermore, we present some exact arguments that various phases including the spin nematic phase and the vector chiral (p-type nematic) phase emerge from an SU(4) symmetric point in the model by the addition of appropriate perturbative interactions. The spin nematic phase generated from the SU(4) point is connected with the spin nematic phase found numerically in the system with only two-spin interactions., Comment: 23 pages with 12 figures

We propose a method to calculate the charge dynamical structure factors for the ground states of correlated electron systems based on the variational Monte Carlo method. Our benchmarks for the one- and two-dimensional Hubbard models show that inclusion of composite-fermion excitations in the basis set greatly improves the accuracy, in reference to the exact charge dynamical structure factors for clusters. Together with examination for larger systems beyond tractable sizes by the exact diagonalization, our results indicate that the variational Monte Carlo method is a promising way for studies on the nature of charge dynamics in correlated materials such as the copper oxide superconductors, if the composite-fermion excitations are properly included in the restricted Hilbert space of intermediate states in the linear response theory. Our results are consistent with the particle-hole excitations inferred from the single-particle spectral function $A(\mathbf{k}, \omega)$ in the literature. We also discuss the importance of incorporating nonlocal composite fermion for more accurate description. Future issues for further improvements are also discussed., Comment: 15 pages, 15 figures

By using the variational Monte Carlo method, we study the magnetization process of the Kitaev honeycomb model in a magnetic field. Our trial wavefunction is a generalized Bardeen-Cooper-Schrieffer wave function with the Jastrow correlation factor, which exactly describes the ground state of the Kitaev model at zero magnetic field using the Jordan-Wigner (JW) transformation. We find that two phase transitions occur for the antiferromagnetic Kitaev coupling, while only one phase transition occurs for the ferromagnetic Kitaev coupling. For the antiferromagnetic Kitaev coupling, we also find that the topology of the momentum distribution of the JW fermions changes at the transition point from the Kitaev spin liquid to an intermediate state. Our numerical results indicate that the intermediate state between the Kitaev spin liquid and the fully polarized phases stably exists in the bulk system on two dimensions for the antiferromagnetic Kitaev coupling against many-body correlations., Comment: 7 pages, 4 figures

Transition metal compounds sometimes exhibit beautiful colors. We report here on a new oxychloride Ca3ReO5Cl2 which shows unusually distinct pleochroism; that is, the material exhibits different colors depending on viewing directions. This ple-ochroism is a consequence of the fact that a complex crystal field splitting of the 5d orbitals of the Re6+ ion in a square-pyramidal coordination of low-symmetry occurs accidentally in the energy range of the visible light spectrum. Since the rele-vant d-d transitions possess characteristic polarization dependences according to the optical selection rule, the orbital states are "visible" in Ca3ReO5Cl2., Comment: 6 pages, 5 figures

We report on the emergence of antiferromagnetic spin chains from two-dimensionally aligned spins on the anisotropic triangular lattice (ATL) in the insulating calcium rhenium oxychloride Ca3ReO5Cl2. The compound contains Re6+ ions each with one unpaired electron in the dxy orbital, which are arranged to form a spin-1/2 ATL with J'/J ~ 0.32 and J = 41 K, where J and J' are magnetic interactions in and between the chains, respectively. In spite of the apparent two dimensionality, we observe clear evidence of a gapless spin liquid that is characteristic of the spin-1/2 Heisenberg chain. This one-dimensionalization must be caused by geometrical frustration: growing antiferromagnetic correlations in every chain effectively cancel out inter-chain zigzag couplings at low temperature. Ca3ReO5Cl2 provides us with a detailed insight into the interesting physics of the ATL antiferromagnet, especially via comparison with the typical ATL compound Cs2CuCl4., Comment: 9 pages, 4 figures, 1 Table

Understanding physics of high-$T_c$ cuprate superconductors remains one of the important problems in materials science. Though a number of diverse theories argue about the superconductivity and competing orders, ab initio and quantitative understanding is lacking. Here, we reproduce the experimental phase diagram of HgBa$_2$CuO$_{4+y}$ by solving its ab initio low-energy effective Hamiltonian without adjustable parameters. It shows a superconducting phase in a wide range of hole density $\delta$, and its competition with charge period-4 plus spin period-8 stripe order near $\delta \sim 0.1$, in agreement with experimental results including recent X-ray scattering. Then a crucial role of off-site interactions in stabilizing the superconductivity is elucidated with emphasis on charge fluctuations. It also clarifies the condensation energy mainly contributed from the onsite Coulomb interaction. The present achievement will enable deeper, predictable understanding on open issues of the high-$T_c$ superconducting mechanism and promote ab initio studies on strongly correlated electrons beyond parametrized model studies.

Three-types (three-band, two-band and one-band) of effective Hamiltonians for the HgBa$_2$CuO$_4$ and three-band effective Hamiltonian for La$_2$CuO$_4$ are derived beyond the level of the constrained-GW approximation combined with the self-interaction correction (cGW-SIC) derived in Hirayama et al. Phys. Rev. B 98, 134501 (2018) by improving the treatment of the interband Hartree energy. The charge gap and antiferromagnetic ordered moment show good agreement with the experimental results when the present effective Hamiltonian is solved, indicating the importance of the present refinement. The obtained Hamiltonians will serve to clarify the electronic structures of these copper oxide superconductors and to elucidate the superconducting mechanism., Comment: 23 pages, 21 figures and supplementary material(22 pages). arXiv admin note: text overlap with arXiv:1708.07498

Asymmetric destruction of the one-third magnetization plateau upon heating is found in the spin-1/2 kagome Heisenberg antiferromagnets using the typical pure quantum state approach. The asymmetry originates from larger density of states of low-lying excited sates of $N_{\rm s}$ spin systems with magnetization $(1/3-2/N_{\rm s})$ than that of low-lying sates with magnetization $(1/3+2/N_{\rm s})$. The enhanced specific heat and entropy that reflect the larger density of states in the lower-field side of the plateau are detectable in candidate materials of the kagome antiferromagnets. We discuss that the asymmetry originates from the unprecedented preservation of the ice rule around the plateau., Comment: 8 pages, 5 figures

mVMC (many-variable Variational Monte Carlo) is an open-source software based on the variational Monte Carlo method applicable for a wide range of Hamiltonians for interacting fermion systems. In mVMC, we introduce more than ten thousands variational parameters and simultaneously optimize them by using the stochastic reconfiguration (SR) method. In this paper, we explain basics and user interfaces of mVMC. By using mVMC, users can perform the calculation by preparing only one input file of about ten lines for widely studied quantum lattice models, and can also perform it for general Hamiltonians by preparing several additional input files. We show the benchmark results of mVMC for the Hubbard model, the Heisenberg model, and the Kondo-lattice model. These benchmark results demonstrate that mVMC provides ground-state and low-energy-excited-state wave functions for interacting fermion systems with high accuracy., Comment: 19 pages, 8 figures, source code can be found at https://ma.issp.u-tokyo.ac.jp/en/app/518 and https://github.com/issp-center-dev/mVMC, accepted for publication in Computer Physics Communications

A three-orbital model derived from the two-dimensional projection of the $ab$ $initio$ Hamiltonian for alkaline doped fullerene A$_3$C$_{60}$ with A=Cs,Rb,K is studied by a variational Monte Carlo method. We correctly reproduce the experimental isotropic s-wave superconductivity around the $ab$ $initio$ parameters. With narrowing the bandwidth, the transition to an insulator is also reproduced, where orbital symmetry is found to be spontaneously broken with emergence of an excitonic Mott insulator for two orbitals and an antiferromagnetic insulator nearly degenerate with a spin liquid for the third orbital. The superconductivity is a consequence of exciton melting., Comment: 10 pages, 10 figures

Ab initio low-energy effective Hamiltonians of two typical high-temperature copper-oxide superconductors, whose mother compounds are La$_2$CuO$_4$ and HgBa$_2$CuO$_4$, are derived by utilizing the multi-scale ab initio scheme for correlated electrons (MACE). The effective Hamiltonians obtained in the present study serve as platforms of future studies to accurately solve the low-energy effective Hamiltonians beyond the density functional theory. It allows further study on the superconducting mechanism from the first principles and quantitative basis without adjustable parameters not only for the available cuprates but also for future design of higher Tc in general. More concretely, we derive effective Hamiltonians for three variations, 1)one-band Hamiltonian for the antibonding orbital generated from strongly hybridized Cu $3d_{x^2-y^2}$ and O $2p_\sigma$ orbitals 2)two-band Hamiltonian constructed from the antibonding orbital and Cu $3d_{3z^2-r^2}$ orbital hybridized mainly with the apex oxygen $p_z$ orbital 3)three-band Hamiltonian consisting mainly of Cu $3d_{x^2-y^2}$ orbitals and two O $2p_\sigma$ orbitals. Differences between the Hamiltonians for La$_2$CuO$_4$ and HgBa$_2$CuO$_4$, which have relatively low and high critical temperatures, respectively, at optimally doped compounds, are elucidated. The main differences are summarized as i) the oxygen $2p_\sigma$ orbitals are farther(~3.7eV) below from the Cu $d_{x^2-y^2}$ orbital for the La compound than the Hg compound(~2.4eV) in the three-band Hamiltonian. This causes a substantial difference in the character of the $d_{x^2-y^2}-2p_\sigma$ antibonding band at the Fermi level and makes the effective onsite Coulomb interaction U larger for the La compound than the Hg compound for the two- and one-band Hamiltonians. ii)The ratio of the second-neighbor to the nearest transfer t'/t is also substantially different (~0.26) for the Hg and ~0.15 for the La compound in the one-band Hamiltonian., Comment: 23 pages, 23 figures and supplementary material(18 pages)

${\mathcal H}\Phi$ [$aitch$-$phi$] is a program package based on the Lanczos-type eigenvalue solution applicable to a broad range of quantum lattice models, i.e., arbitrary quantum lattice models with two-body interactions, including the Heisenberg model, the Kitaev model, the Hubbard model and the Kondo-lattice model. While it works well on PCs and PC-clusters, ${\mathcal H}\Phi$ also runs efficiently on massively parallel computers, which considerably extends the tractable range of the system size. In addition, unlike most existing packages, ${\mathcal H}\Phi$ supports finite-temperature calculations through the method of thermal pure quantum (TPQ) states. In this paper, we explain theoretical background and user-interface of ${\mathcal H}\Phi$. We also show the benchmark results of ${\mathcal H}\Phi$ on supercomputers such as the K computer at RIKEN Advanced Institute for Computational Science (AICS) and SGI ICE XA (Sekirei) at the Institute for the Solid State Physics (ISSP)., Comment: 15 pages, 8 figures

Finite-temperature properties of the frustrated Hubbard model are theoretically examined by using the recently proposed thermal pure quantum state, which is an unbiased numerical method for finite-temperature calculations. By performing systematic calculations for the frustrated Hubbard model, we show that the geometrical frustration controls the characteristic energy scale of the metal-insulator transitions. We also find that entropy remains large even at moderately high temperature around the region where the quantum spin liquid is expected to appear at zero temperature. We propose that this is a useful criterion whether the target systems have a chance to be the quantum spin liquid or the non-magnetic insulator at zero temperature., Comment: 5 pages, 4 figures, code can be found at http://ma.cms-initiative.jp/en/application-list/hphi, v2: Fig.4 is updated

Stabilizing superconductivity at high temperatures and elucidating its mechanism have long been major challenges of materials research in condensed matter physics. Meanwhile, recent progress in nanostructuring offers unprecedented possibilities for designing novel functionalities. Above all, thin films of cuprate and iron-based high-temperature superconductors exhibit remarkably better superconducting characteristics (e.g. higher critical temperatures) than in the bulk, but the underlying mechanism is still not understood. Solving microscopic models suitable for cuprates, here, we demonstrate that at an interface between a Mott insulator and an overdoped non-superconducting metal, the superconducting amplitude stays always pinned at the optimum achieved in the bulk, independently of the carrier concentration in the metal. This is in contrast to the dome-like dependence in bulk superconductors, but consistent with the astonishing independence of the critical temperature from the carrier density x observed at interfaces of La2CuO4 and La2-xSrxCuO4. We furthermore identify a self-organization mechanism as responsible for the pinning at the optimum amplitude: An emergent electronic structure induced by interlayer phase separation eludes bulk phase separation and inhomogeneities that would kill superconductivity in the bulk. Thus, interfaces provide an ideal tool to enhance and stabilize superconductivity. This interfacial example opens up further ways of shaping superconductivity by suppressing competing instabilities, with direct perspectives for designing devices., Comment: 27 pages, 5 figures

A new computational method for finite-temperature properties of strongly correlated electrons is proposed by extending the variational Monte Carlo method originally developed for the ground state. The method is based on the path integral in the imaginary-time formulation, starting from the infinite-temperature state that is well approximated by a small number of certain random initial states. Lower temperatures are progressively reached by the imaginary-time evolution. The algorithm follows the framework of the quantum transfer matrix and finite-temperature Lanczos methods, but we extends them to treat much larger system sizes without the negative sign problem by optimizing the truncated Hilbert space on the basis of the time-dependent variational principle (TDVP). This optimization algorithm is equivalent to the stochastic reconfiguration (SR) method that has been frequently used for the ground state to optimally truncate the Hilbert space. The obtained finite-temperature states allow an interpretation based on the thermal pure quantum (TPQ) state instead of the conventional canonical-ensemble average. Our method is tested for the one- and two-dimensional Hubbard models and its accuracy and efficiency are demonstrated., Comment: 13 pages, 9 figures, plus appendix

Quantum tricriticality of a $J_1$-$J_2$ antiferromagnetic Ising model on a square lattice is studied using the mean-field (MF) theory, scaling theory, and the unbiased world-line quantum Monte-Carlo (QMC) method based on the Feynman path integral formula. The critical exponents of the quantum tricritical point (QTCP) and the qualitative phase diagram are obtained from the MF analysis. By performing the unbiased QMC calculations, we provide the numerical evidence for the existence of the QTCP and numerically determine the location of the QTCP in the case of $J_1=J_2$. From the systematic finite-size scaling analysis, we conclude that the QTCP is located at $H_{\rm QTCP}/J_1=3.260(2)$ and $\Gamma_{\rm QTCP}/J_1=4.10(5)$. We also show that the critical exponents of the QTCP are identical to those of the MF theory because the QTCP in this model is in the upper critical dimension. The QMC simulations reveal that unconventional proximity effects of the ferromagnetic susceptibility appear close to the antiferromagnetic QTCP, and the proximity effects survive for the conventional quantum critical point. We suggest that the momentum dependence of the dynamical and static spin structure factors is useful for identifying the QTCP in experiments., Comment: 12 pages, 9 figures

The iron chalcogenides FeTe and FeSe belong to the family of iron-based superconductors. We study the magnetism in these compounds in the normal state using the ab initio downfolding scheme developed for strongly correlated electron systems. In deriving ab initio low-energy effective models, we employ the constrained GW method to eliminate the double counting of electron correlations originating from the exchange correlations already taken into account in the density functional theory. By solving the derived ab initio effective models, we reveal that the elimination of the double counting is important in reproducing the bicollinear antiferromagnetic order in FeTe, as is observed in experiments. We also show that the elimination of the double counting induces a unique degeneracy of several magnetic orders in FeSe, which may explain the absence of the magnetic ordering. We discuss the relationship between the degeneracy and the recently found puzzling phenomena in FeSe as well as the magnetic ordering found under pressure., Comment: 10 pages, 7 figures, 5 tables