arXiv subjects

Masatoshi Imada

Publications and source records attributed to Masatoshi Imada.

At least 19 recordsLinked to original sources

arXiv2026

Microscopic mechanism of high-temperature superconductivity revealed by ab initio studies on hole-doped multilayer cuprates HgBa$_2$Ca$_2$Cu$_3$O$_8$ under pressure

Triple-layer cuprate superconductor $\mathrm{HgBa_2Ca_2Cu_3O_8}$ (Hg1223) keeps the record of the highest superconducting (SC) critical temperature $T_{c}\sim 134$K among all the existing materials at ambient pressure. $T_{c}$ further increases under pressure up to $T_{c}\sim 160$K. However, its microscopic mechanism remains to be elucidated. We solve {\it ab initio} Hamiltonians for Hg1223 using a variational solver supplemented by a neural network. The pressure dependence of the $d$-wave SC order parameter and estimated $T_{c}$ show a $T_{\mathrm{c}}$ peak around 30GPa in quantitative agreement with the experiments. The origin of the strong SC amplitude at ambient pressure is identified as strong local Coulomb repulsion $U$ attributed to poor screening. Further increase in $T_{c}$ under pressure is understood from interplay of three elements, namely increased electron hopping $t$, decreased $U$ and more importantly, strongly reduced offsite Coulomb repulsion $V$ with increasing pressure. Pairing mechanism is identified as the emergent local attraction counterintuitively generated from the originally strong local repulsion $U$. The emergent attraction is interpreted from ``attraction from reduced repulsion'', originating from the release of the fluctuating doubly-occupied sites characterized from the ``false vacuum'' in the Mott insulator to the double-occupation-free $d$-wave SC states upon carrier doping. This instantaneous attraction is in contrast with the conventional BCS SC mediated by bosonic glues. The local attraction is consistent with the electron fractionalization supported in experimental analyses. The coexistence of the SC and antiferromagnetic order is also demonstrated as a characteristic feature of the multilayer system. The microscopic understanding of Hg1223 offers a new route explicitly using this emergent attraction to design and optimize SC materials.

cond-mat.supr-con↗

arXiv2025

Unified description of cuprate superconductors by fractionalized electrons emerging from integrated analyses of photoemission spectra and quasiparticle interference

Electronic structure of high-temperature superconducting cuprates is studied by analyzing experimental data independently obtained from two complementary spectroscopies, one, quasiparticle interference (QPI) measured by scanning-tunneling microscopy and the other, angle-resolved photoemission spectroscopy (ARPES) and by combining these two sets of data in a unified theoretical analysis. Through explicit calculations of experimentally measurable quantities, we show that a simple two-component fermion model (TCFM) representing electron fractionalization succeeds in reproducing various detailed features of these experimental data: ARPES and QPI data are concomitantly reproduced by the TCFM in full energy and momentum spaces. The measured QPI pattern reveals a signature characteristic of the TCFM, distinct from the conventional single-component prediction, supporting the validity of the electron fractionalization in the cuprate. The integrated analysis also solves the puzzles of ARPES and QPI data that are seemingly inconsistent with each other. The overall success of the TCFM offers a comprehensive understanding of the electronic structure of the cuprates. We further predict that a characteristic QPI pattern should appear in the unoccupied high-energy part if the fractionalization is at work. We propose that integrated-spectroscopy analyses offer a promising way to explore challenging issues of strongly correlated electron systems.

cond-mat.str-el↗

arXiv2024

Quantum many-body solver using artificial neural networks and its applications to strongly correlated electron systems

With the evolution of numerical methods, we are now aiming at not only qualitative understanding but also quantitative prediction and design of quantum many-body phenomena. As a novel numerical approach, machine learning techniques have been introduced in 2017 to analyze quantum many-body problems. Since then, proposed various novel approaches have opened a new era, in which challenging and fundamental problems in physics can be solved by machine learning methods. Especially, quantitative and accurate estimates of material-dependent physical properties of strongly correlated matter have now become realized by combining first-principles calculations with highly accurate quantum many-body solvers developed with the help of machine learning methods. Thus developed quantitative description of electron correlations will constitute a key element of materials science in the next generation.

cond-mat.str-el↗

arXiv2024

Fermi Machine -- Quantum Many-Body Solver Derived from Correspondence between Noninteracting and Strongly Correlated Fermions

Stimulated by the successful descriptions of strongly correlated electron systems by fractionalized fermions, correspondence between interacting fermions and non-interacting multi-component fermions is formulated in examples of the Hubbard model. The formalism enables constructions of the neural network for a quantum many-body solver represented by coupled noninteracting fermions. After showing the exact correspondence of 1- and 2-site Hubbard model to two-component noninteracting fermions, numerical algorithm of the quantum machine learning for the Hubbard model is proposed. Benchmark for the 4-site systems is successfully presented and promising future directions as well as implications are discussed.

cond-mat.str-el↗

arXiv2024

Forecasting long-time dynamics in quantum many-body systems by dynamic mode decomposition

Reliable numerical computation of quantum dynamics is a fundamental challenge when the long-ranged quantum entanglement plays essential roles as in the cases governed by quantum criticality in strongly correlated systems. Here we apply a method that utilizes reliable short-time data of physical quantities to accurately forecast long-time behavior of the strongly entangled systems. We straightforwardly employ the simple dynamic mode decomposition (DMD), which is commonly used in fluid dynamics. Despite the simplicity of the method, the effectiveness and applicability of the DMD in quantum many-body systems such as the Ising model in the transverse field at the critical point are demonstrated, even when the time evolution at long time exhibits complicated features such as a volume-law entanglement entropy and consequential power-law decays of correlations characteristic of systems with long-ranged quantum entanglements unlike fluid dynamics. The present method, though simple, enables accurate forecasts amazingly at time as long as nearly an order of magnitude longer than that of the short-time training data. Effects of noise on the accuracy of the forecast are also investigated, because they are important especially when dealing with the experimental data. We find that a few percentages of noise do not affect the prediction accuracy destructively.

quant-ph↗

arXiv2023

Dome structure in pressure dependence of superconducting transition temperature for HgBa$_2$Ca$_2$Cu$_3$O$_8$ -- Studies by $ab$ $initio$ low-energy effective Hamiltonian

The superconducting (SC) cuprate HgBa$_2$Ca$_2$Cu$_3$O$_8$ (Hg1223) has the highest $T_{c}^{\rm opt}\simeq 138$ K (the experimental SC transition temperature at optimal hole doping) among cuprates at ambient pressure $P_{\rm amb}$. $T_{c}^{\rm opt}$ increases under pressure $P$ and reaches $164$ K at $P_{\rm opt}\simeq 30$ GPa, then decreases with increasing $P>P_{\rm opt}$. To understand the microscopic origin of this dome-like $P$ dependence of $T_{c}^{\rm opt}$, we consider the $ab$ $initio$ low-energy effective Hamiltonian (LEH) for the antibonding (AB) Cu$3d_{x^2-y^2}$/O$2p_{\sigma}$ band. In the AB LEH for cuprates with $N_\ell \leq 2$ laminated CuO$_2$ planes between block layers, it was proposed that $T_{c}^{\rm opt}\simeq 0.16|t_1|F_{\rm SC}$, where $t_1$ is the nearest neighbor hopping and the SC order parameter $F_{\rm SC}$ at optimal hole doping mainly depends on $u=U/|t_1|$ ($U$ is the onsite effective Coulomb repulsion): $F_{\rm SC}$ is maximal at $u_{\rm opt}\simeq 8.5$ and decreases sharply with decreasing $u$ for $u P_{\rm opt}$, the decrease in $T_{c}^{\rm opt}$ is accounted for by (II): The rapid decrease in $F_{\rm SC}$ with decreasing $u$ for $u<u_{\rm opt}$ dominates over (I). We support (A,B) based on studies of other cuprates.

cond-mat.supr-con↗

arXiv2023

Ground state of the $S$=1/2 pyrochlore Heisenberg antiferromagnet: A quantum spin liquid emergent from dimensional reduction

The quantum antiferromagnet on the pyrochlore lattice offers an archetypal frustrated system, which potentially realizes a quantum spin liquid characterized by the absence of standard spontaneous symmetry breaking even at zero temperature, unusually as an isotropic 3D system. Despite tremendous progress in the literature, however, the nature of the ground state of the fully quantum-mechanical spin Hamiltonian on the pyrochlore lattice still remains elusive. Here, we show that an unconventional type of quantum spin liquid is born out from the pyrochlore system after the self-organized dimensional reduction leading to confined states in 2D layers. This conclusion is obtained from state-of-the-art variational Monte Carlo (VMC) simulations at zero temperature. Quantum spin liquids triggered by the emergent dimensional reduction is an unexplored route of the spin-liquid formation. The dimensional reduction from 3D to 2D is a consequence of a conventional spontaneous symmetry breaking, while the resultant decoupling of layers enables the emergence of a 2D quantum spin liquid that is adiabatically disconnected from trivial product states and exhibits strong quantum entanglement. The stabilized quantum spin liquid exhibits an algebraic decay of correlations and vanishing excitation gap in the thermodynamic limit. The wave-function structure supports the fractionalization of the spin into spinons. This spin-liquid ground state persists in the presence of spin-orbit interactions, which expands the possibilities of realizing quantum spin liquids in real pyrochlore-structured materials.

cond-mat.str-el↗

arXiv2023

Superconductivity studied by solving ab initio low-energy effective Hamiltonians for carrier doped CaCuO$_2$, Bi$_2$Sr$_2$CuO$_6$, Bi$_2$Sr$_2$CaCu$_2$O$_8$, and HgBa$_2$CuO$_4$

We numerically analyze superconductivity (SC) in the cuprate superconductors by using ab initio effective Hamiltonians consisting of the antibonding combination of Cu $3d_{x^2-y^2}$ and O $2p_{\sigma}$ orbitals. We perform variational Monte Carlo calculations for the four carrier doped cuprates with diverse experimental optimal SC critical temperature $T_{c}^{\rm opt}$: CaCuO$_2$ ($T_{c}^{\rm opt} \sim 110$ K), Bi$_2$Sr$_2$CuO$_6$ ($T_{c}^{\rm opt} \sim 10$-$40$ K), Bi$_2$Sr$_2$CaCu$_2$O$_8$ ($T_{c}^{\rm opt} \sim 85$-$100$ K), and HgBa$_2$CuO$_4$ ($T_{c}^{\rm opt} \sim 90$ K). Materials and hole doping concentration ($\delta$) dependencies of the SC order parameter $F_{\rm SC}$ and the competition with spin/charge order show essential and quantitative agreements with the available experiments in the following points: (1) The ground state is commonly the SC state, which is severely competing with the charge/spin stripe and antiferromagnetic states. (2) $F_{\rm SC}$ shows amplitude consistent with the superfluid density measured in the muon spin resonance and its dome structure found in $\delta$ dependence shows consistency with that of the SC gap in the tunneling and photoemission measurements. We further find insights into the universal SC mechanism: (I) $F_{\rm SC}$ increases with the ratio $U/|t_1|$, indicating that $U/|t_1|$ is the principal component controlling the SC. Here, $U$ and $t_1$ are the onsite Coulomb repulsion and the nearest neighbor hopping, respectively, in the Hamiltonians. (II) A universal scaling $T_{c}^{\rm opt}\sim 0.16 \lvert t_1 \rvert F_{\rm SC}$ holds. (III) SC is enhanced and optimized if $U$ is increased beyond the real available materials. It is further enhanced by decreasing the offsite interaction. The present findings provide useful clues for the design of new SC materials with even higher $T_{c}^{\rm opt}$.

cond-mat.supr-con↗

arXiv2023

Quantum criticality of bandwidth-controlled Mott transition

Metallic states near the Mott insulator show a variety of quantum phases including various magnetic, charge ordered states and high-temperature superconductivity in various transition metal oxides and organic solids. The emergence of a variety of phases and their competitions are likely intimately associated with quantum transitions between the electron-correlation driven Mott insulator and metals characterized by its criticality, and is related to many central questions of condensed matter. The quantum criticality is, however, not well understood when the transition is controlled by the bandwidth through physical parameters such as pressure. Here, we quantitatively estimate the universality class of the transition characterized by a comprehensive set of critical exponents by using a variational Monte Carlo method implemented as an open-source innovated quantum many-body solver, with the help of established scaling laws at a typical bandwidth-controlled Mott transition. The criticality indicates a weaker charge and density instability in contrast to the filling-controlled transition realized by carrier doping, implying a weaker instability to superconductivity as well. The present comprehensive clarification opens up a number of routes for quantitative experimental studies for complete understanding of elusive quantum Mott transition and nearby strange metal that cultivate future design of functionality.

cond-mat.str-el↗

arXiv2023

Hidden self-energies as origin of cuprate superconductivity revealed by machine learning

Experimental data are the source of understanding matter. However, measurable quantities are limited and theoretically important quantities are sometimes hidden. Nonetheless, recent progress of machine-learning techniques opens possibilities of exposing them only from available experimental data. In this paper, after establishing the reliability of the method in various careful benchmark tests, the Boltzmann-machine method is applied to the angle-resolved photoemission spectroscopy spectra of cuprate high temperature superconductors, Bi$_2$Sr$_2$CuO$_{6+δ}$ (Bi2201) and Bi$_2$Sr$_2$CaCuO$_{8+δ}$ (Bi2212). We find prominent peak structures both in normal and anomalous self-energies, but they cancel in the total self-energy making the structure apparently invisible, while the peaks make universally dominant contributions to superconducting gap, hence evidencing the signal that generates the high-$T_{\rm c}$ superconductivity. The relation between superfluid density and critical temperature supports involvement of universal carrier relaxation associated with dissipative strange metals, where enhanced superconductivity is promoted by entangled quantum-soup nature of the cuprates. The present achievement opens avenues for innovative machine-learning spectroscopy method to reveal fundamental properties hidden in direct experimental accesses.

cond-mat.str-el↗

arXiv2023

Variational Benchmarks for Quantum Many-Body Problems

The continued development of computational approaches to many-body ground-state problems in physics and chemistry calls for a consistent way to assess its overall progress. In this work, we introduce a metric of variational accuracy, the V-score, obtained from the variational energy and its variance. We provide an extensive curated dataset of variational calculations of many-body quantum systems, identifying cases where state-of-the-art numerical approaches show limited accuracy, and future algorithms or computational platforms, such as quantum computing, could provide improved accuracy. The V-score can be used as a metric to assess the progress of quantum variational methods toward a quantum advantage for ground-state problems, especially in regimes where classical verifiability is impossible.

quant-ph↗

arXiv2022

$Ab$ $initio$ low-energy effective Hamiltonians for high-temperature superconducting cuprates Bi$_2$Sr$_2$CuO$_6$, Bi$_2$Sr$_2$CaCu$_2$O$_8$, HgBa$_2$CuO$_4$ and CaCuO$_2$

We derive $ab$ $initio$ low-energy effective Hamiltonians (LEH) for high-temperature superconducting (SC) copper oxides Bi$_2$Sr$_2$CuO$_6$ (Bi2201, $N_{\ell}=1$, $T_c^{\rm exp} \sim 10$ K), Bi$_2$Sr$_2$CaCu$_2$O$_8$ (Bi2212, $N_{\ell}=2$, $T_c^{\rm exp} \sim 84$ K), HgBa$_2$CuO$_4$ (Hg1201, $N_{\ell}=1$, $T_c^{\rm exp} \sim 90$ K) and CaCuO$_2$ (Ca11, $N_{\ell}=\infty$, $T_c^{\rm exp} \sim 110$ K), with different experimental optimal SC transition temperature $T_c^{\rm exp}$ and number $N_{\ell}$ of laminated CuO$_2$ planes between the two neighboring block layers. We apply the latest methodology of the multiscale $ab$ $initio$ scheme for correlated electron systems (MACE), and focus on the LEH consisting of one antibonding (AB) Cu$3d_{x^2-y^2}$/O$2p_σ$ orbital centered on each Cu atom. We discuss prominent features of this LEH: (1) The ratio $U/|t_1|$ between the onsite effective Coulomb repulsion (ECR) $U$ and amplitude of nearest neighbour hopping $t_1$ increases with $T^{\rm exp}_c$ and $N_{\ell}$, consistently with the expected increase in $d$-wave SC correlation function $P_{dd}$ with $U/|t_1|$. One possible cause of the increase of $U/|t_1|$ is the replacement of apical O atoms by Cu atoms from neighbouring CuO$_2$ planes when $N_{\ell}$ increases. Furthermore, we show that the increase in distance between Cu and apical O atoms decreases the effective screening (ES) by electrons outside of the LEH and increases $U/|t_1|$. (2) For Hg1201 and Ca11, we show that $U/|t_1|$ decreases when hole doping per AB orbital $δ$ increases, which may partly account for the disappearance of SC when $δ$ exceeds the optimal value in experiment. (3) For $N_{\ell} \geq 2$, off-site inter-CuO$_2$ plane ECR is comparable to off-site intra-CuO$_2$ plane ECR. We discuss contributions of inter-CuO$_2$ plane ECR to both $P_{dd}$ and the stability of the SC state.

cond-mat.str-el↗

arXiv2022

$Ab$ $initio$ material design of Ag-based oxides for high-$T_c$ superconductor

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.

cond-mat.supr-con↗

arXiv2022

Quantum mechanically driven structural-spin glass in two dimensions at finite temperature

In magnetic materials, spins sometimes freeze into spatially disordered glassy states. Glass forming liquids or structural glasses are found very often in three dimensions. However, in two dimensions(2D) it is believed that both spin glass and structural glass can never exist at a finite temperature because they are destroyed by thermal fluctuations. Using a large-scale quantum Monte Carlo simulation, we discover a quantum-mechanically driven 2D glass phase at finite temperatures. Our platform is an Ising spin model with a quantum transverse field on a frustrated triangular lattice. How the present glass phase is formed is understood by the following three steps. First, by the interplay of geometrical frustration and quantum fluctuation, part of the spins spontaneously form an antiferromagnetic honeycomb spin-superstructure. Then, small randomness in the bond interaction works as a relevant perturbation to this superstructure and breaks it up into {\it domains}, making it a structural glass. The glassiness of the superstructure, in turn, generates an emergent random magnetic field acting on the remaining fluctuating spins and freezes them. The shape of domains thus formed depends sensitively on the quenching process, which is one of the characteristic features of glass, originating from a multi-valley free-energy landscape. The present system consists only of {\it a single} bistable Ising degree of freedom, which naturally does not become a structural glass alone nor a spin glass alone. Nevertheless, a glass having both types of nature emerges in the form of coexisting two-component glasses, algebraic structural-glass and long-range ordered spin-glass. This new concept of glass-forming mechanism opens a way to realize functional glasses even in low dimensional systems.

cond-mat.dis-nn↗

arXiv2022

Optimized Implementation for Calculation and Fast-Update of Pfaffians Installed to the Open-Source Fermionic Variational Solver mVMC

In this article, we present a high performance, portable and well templated implementation for computing and fast-updating Pfaffian and inverse of an even-ranked skew-symmetric (antisymmetric) matrix. It is achieved with a skew-symmetric, blocked variant of the Parlett-Reid algorithm and a blocked update scheme based on the Woodbury matrix identity. Installation of this framework into the geminal-wavefunction-based many-variable Variational Monte Carlo (mVMC) code boosts sampling performance to up to more than $6$ times without changing Markov chain's behavior. The implementation is based on an extension of the BLAS-like instantiation software (BLIS) framework which has optimized kernel for many state-of-the-art processors including Intel Skylake-X, AMD EPYC Rome and Fujitsu A64FX.

physics.comp-ph↗

arXiv2022

Unconventional dual 1D-2D quantum spin liquid revealed by $ab$ $initio$ studies on organic solids family

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 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.

cond-mat.str-el↗

arXiv2021

Order-$N$ orbital-free density-functional calculations with machine learning of functional derivatives for semiconductors and metals

Orbital-free density functional theory (OFDFT) offers a challenging way of electronic-structure calculations scaled as $\mathcal{O}(N)$ computation for system size $N$. We here develop a scheme of the OFDFT calculations based on the accurate and transferrable kinetic-energy density functional (KEDF) which is created in an unprecedented way using appropriately constructed neural network (NN). We show that our OFDFT scheme reproduces the electron density obtained in the state-of-the-art DFT calculations and then provides accurate structural properties of 24 different systems, ranging from atoms, molecules, metals, semiconductors and an ionic material. The accuracy and the transferability of our KEDF is achieved by our NN training system in which the kinetic-energy functional derivative (KEFD) at each real-space grid point is used. The choice of the KEFD as a set of training data is essentially important, because first it appears directly in the Euler equation which one should solve and second, its learning assists in reproducing the physical quantity expressed as the first derivative of the total energy. More generally, the present development of KEDF $T[ρ]$ is in the line of systematic expansion in terms of the functional derivatives $δ^{\ell_1} T/δρ^{\ell_1}$ through progressive increase of $\ell_1$. The present numerical success demonstrates the validity of this approach. The computational cost of the present OFDFT scheme indeed shows the $\mathcal{O}(N)$ scaling, as is evidenced by the computations of the semiconductor SiC used in power electronics.

physics.comp-ph↗

arXiv2021

Magnetization Step in Spatially Distorted Heisenberg Kagome Antiferromagnets

Motivated by a recent experiment on volborthite, a typical spin-$1/2$ antiferromagnet with a kagomé lattice structure, we study the magnetization process of a classical Heisenberg model on a spatially distorted kagomé lattice using the Monte Carlo (MC) method. We find a distortion-induced magnetization step at low temperatures and low magnetic fields. The magnitude of this step is given by $Δm_z=\left|1-α\right|/3α$ at zero temperature, where $α$ denotes the spatial anisotropy in exchange constants. The magnetization step signals a first-order transition at low temperatures, between two phases distinguished by distinct and well-developed short-range spin correlations, one characterized by spin alignment of a local $120^{\circ}$ structure with a $\sqrt{3}\times\sqrt{3}$ period, and the other by a partially spin-flopped structure. We point out the relevance of our results to the unconventional steps observed in volborthite.

cond-mat.str-el↗