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Yuta Murakami

Publications and source records attributed to Yuta Murakami.

At least 19 recordsLinked to original sources

Prominent Dimensional Effects on High-order Harmonic Generation in Strongly Correlated Electron Systems

Dimensionality strongly affects elementary excitations in correlated quantum materials, yet its impact on extreme nonlinear optical responses remains largely unexplored. Here, we combine high-harmonic generation (HHG) experiments on quasi-one-dimensional SrCuO$_2$ and quasi-two-dimensional Pr$_2$CuO$_4$ with nonequilibrium simulations of Hubbard models. We find a pronounced dimensional contrast: SrCuO$_2$ exhibits a robust plateau-like high-harmonic spectrum with weak temperature dependence, whereas Pr$_2$CuO$_4$ shows a monotonic decrease in harmonic yield and strong thermal suppression, especially at higher harmonics. The simulations qualitatively reproduce these trends and identify dimensionality-dependent doublon--holon dephasing, governed by spin--charge coupling, as their microscopic origin. These results establish dimensionality and spin--charge coupling as key control parameters for extreme nonlinear optical responses in correlated insulators.

cond-mat.str-el

Generalized Keldysh formalism for nonequilibrium correlation functions and its application to fluctuation dynamics

Recent advances in time-resolved spectroscopies provide increasing access to collective dynamics in correlated quantum materials. However, computing the corresponding nonequilibrium two-particle correlation functions remains a major challenge. Here, by introducing a contour-dependent virtual probe field within the generalized Keldysh formalism, we propose an approach that computes such correlation functions with the vertex corrections essential for describing collective dynamics. In particular, we introduce a linear integral equation that computes the correlation functions without explicitly constructing the four-time vertex kernel, and develop its matrix-free Krylov solver based on quantics tensor trains. Combining our method with nonequilibrium dynamical mean-field theory, we show that the fluctuation dynamics of the order parameter in a nonequilibrium symmetry-broken state depends significantly on whether vertex corrections are included, and that the fluctuation and its decay time grow near the nonthermal critical point. Our approach thus provides a practical route for evaluating nonequilibrium correlation functions, which are emerging as key observables for characterizing states far from equilibrium.

cond-mat.str-el

NESSi 2.0: The Non-Equilibrium Systems Simulation package version 2.0

Nonequilibrium Green's functions provide a powerful framework for studying quantum many-body dynamics including the laser-induced dynamics in solids. The Non-Equilibrium Systems Simulation package (NESSi) offers an efficient platform for such simulations, ranging from perturbative approaches like nonequilibrium $GW$ to nonequilibrium dynamical mean-field theory. However, simulations based on nonequilibrium Green's functions become computationally demanding when the dynamics span a large temporal range, such as from sub-femtosecond electron dynamics to the picosecond dynamics of collective modes. Due to the memory integral in the Kadanoff-Baym equations, which serve as equations of motion for nonequilibrium Green's functions, the computational cost scales as $\mathcal{O}(N_t^3)$ with the number of timesteps $N_t$, and the memory requirement scales as $\mathcal{O}(N_t^2)$. In this work, we extend NESSi by incorporating techniques that aim to overcome this bottleneck: (i) By truncating the memory integrals in the KBE to a maximum of $N_c$ timesteps, the computational complexity is reduced to $\mathcal{O}(N_tN_c^2)$, and the memory requirement to $\mathcal{O}(N_c^2)$. Provided that the results converge with respect to the cutoff $N_c$, memory truncation allows to extend the simulations to significantly longer times. (ii) We introduce functionalities to describe nonequilibrium steady states, i.e. time-translationally invariant nonequilibrium states. Such states are relevant for transport settings, and they provide an approximate description of slowly evolving (prethermal) nonequilibrium states.

cond-mat.str-el

Photoemission Signatures of Photoinduced Carriers and Excitons in One-Dimensional Mott Insulators

We theoretically study photoemission spectra for photodoped one-dimensional Mott insulators that can host excitons, and show that their spectral characteristics differ qualitatively from those of photodoped semiconductors. In conventional semiconductors, photoemission spectra are well understood; free charge carriers generate spectral weight near the bottom of the conduction band, while the formation of excitons leads to replica features of the valence band appearing inside the band gap. In one-dimensional Mott insulators, on the other hand, strong correlations give rise to fractionalized elementary excitations-spinons, holons, and doublons-which fundamentally modify the photoemission response. We find that when photodoped carriers, i.e., doublons and holons, remain unbound, the photoemission spectrum directly reflects the dispersion of spinons, i.e., magnetic elementary excitations. In contrast, when a doublon and a holon form an excitonic bound state, replica structures of the lower Hubbard band emerge inside the Mott gap, carrying contributions from both spinon and holon excitations. Importantly, the distribution of the in-gap signal depends sensitively on the degree of doublon-holon binding. The origin of these spectral features is clarified through a combination of exact diagonalization and the slave-particle approach. These results indicate that photoemission from photoinduced carriers and excitons in strongly correlated electron systems can provide information on magnetic properties and carrier-binding properties.

cond-mat.str-el

Excitonic correlations in the equilibrium and voltage-biased bilayer Hubbard model: multi-orbital two-particle self-consistent approach

We develop a nonequilibrium multi-orbital extension of the two-particle self-consistent theory and apply it to the bilayer Hubbard model as a minimal platform to investigate correlation effects in the presence of interlayer interactions and tunneling. The method determines vertex corrections in the spin and charge channels self-consistently at the two-particle level, thereby avoiding the spurious finite-temperature phase transitions that limit dynamical mean-field theory in two dimensions. We derive the spectral self-energy and implement the framework directly on the real-frequency axis within the Keldysh nonequilibrium Green's function formalism, enabling the treatment of both equilibrium and non-equilibrium steady states without relying on numerical analytic continuation. As an application, we demonstrate that a pseudogap can emerge in the bilayer Hubbard model when spin, charge, or excitonic fluctuations become sufficiently strong. Instabilities in different channels are also evaluated in an unbiased manner across the parameter space. Remarkably, we find that the excitonic susceptibility grows with increasing interlayer bias, before it gets suppressed at large biases by the charge imbalance between the layers. This work establishes a versatile and computationally efficient framework for investigating correlated multi-orbital systems under nonequilibrium conditions.

cond-mat.str-el

High-harmonic generation during ultrafast melting of a Mott insulating state

Solids in an intense laser field show high-harmonic generation (HHG), which can provide information on carrier dynamics and band structures in weakly correlated systems. In strongly correlated systems, a laser field can induce a transition between the various electronic phases formed by the entanglement of charge, spin, and orbital degrees of freedom via carrier generation. The HHG accompanying this process can reflect information on the nonequilibrium electronic-state dynamics along the oscillating field-an aspect that remains unresolved to date. Here, we show that an intense mid-infrared (MIR) pulse induces melting of a Mott-insulator state in a one-dimensional cuprate, Sr2CuO3, the evolution of which leaves a trace in the HH spectra. When the electric-field amplitude exceeds 6 MV/cm, carriers are efficiently generated and each harmonic frequency decreases from odd multiples of the MIR frequency. Dynamical mean-field theory (DMFT) presents a possibility that these redshifts originate from a series of electronic-structure reconstructions in each electric-field cycle during the melting of the Mott-insulator state, which modifies the radiation phase from carrier recombination cycle-by-cycle. This phenomenon is negligible in rigid-band systems. This experimental-theoretical study suggests that HH spectroscopy has the potential to obtain information on the cycle-by-cycle dynamics of nonequilibrium transitions in correlated materials.

cond-mat.str-el

Charge creation via quantum tunneling in one-dimensional Mott insulators: A numerical study of the extended Hubbard model

Charge creation via quantum tunneling, i.e. dielectric breakdown, is one of the most fundamental and significant phenomena arising from strong light(field)-matter coupling. In this work, we conduct a systematic numerical analysis of quantum tunneling in one-dimensional Mott insulators described by the extended ($U$-$V$) Hubbard model. We discuss the applicability of the analytical formula for doublon-holon (DH) pair production, previously derived for the one-dimensional Hubbard model, which highlights the relationship between the tunneling threshold, the charge gap, and the correlation length. We test the formulas ability to predict both DH pair production and energy increase rate. Using tensor-network-based approaches, we demonstrate that the formula provides accurate predictions in the absence of excitonic states facilitated by the nearest-neighbor interaction $V$. However, when excitonic states emerge, the formula more accurately describes the rate of energy increase than the DH pair creation rate and in both cases gets improved by incorporating the exciton energy as the effective gap.

cond-mat.str-el

Optical signatures of dynamical excitonic condensates

We theoretically study dynamical excitonic condensates occurring in bilayers with an imposed chemical potential difference and in photodoped semiconductors. We show that optical spectroscopy can experimentally identify phase-trapped and phase-delocalized dynamical regimes of condensation. In the weak-bias regime, the trapped dynamics of the order parameter's phase lead to an in-gap absorption line at a frequency almost independent of the bias voltage, while for larger biases, the frequency of the spectral feature increases approximately linearly with bias. In both cases there is a pronounced second harmonic response. Close to the transition between the trapped and freely oscillating states, we find a strong response upon application of a weak electric probe field and compare the results to those found in a minimal model description for the dynamics of the order parameter's phase and analyze the limitations of the latter.

cond-mat.str-el

High harmonic generation in altermagnets

We study high harmonic generation in altermagnetic metals with and without spin-orbit coupling. The altermagnetism manifests itself in the magnetic field dependence of the low harmonics associated with intra-band dynamics. Spin-orbit coupling leads to additional higher energy peaks and plateau structures originating from inter-band transitions. While the pure altermagnet or spin-orbit system exhibits no circular dichroism in the high-harmonic response, an altermagnetic system with spin-orbit coupling shows such a dichroism. We also analyze the spin currents and their high harmonic spectrum.

cond-mat.mes-hall

Many-body effects on high-harmonic generation in Hubbard ladders

We show how many-body effects associated with background spin dynamics control the high-harmonic generation (HHG) in Mott insulators by analyzing the two-leg ladder Hubbard model. Spin dynamics activated by the interchain hopping $t_y$ drastically modifies the HHG features. When two chains are decoupled ($t_y=0$), HHG originates from the dynamics of coherent doublon-holon pairs because of spin-charge separation. With increasing $t_y$, the doublon-holon pairs lose their coherence due to their interchain hopping and resultant spin-strings. Furthermore, the HHG signal from spin-polarons -- charges dressed by spin clouds -- leads to an additional plateau in the HHG spectrum. For large $t_y$, we identify unconventional HHG processes involving $three$ elementary excitations -- two polarons and one magnon. Our results demonstrate the nontrivial nature of HHG in strongly correlated systems, and its qualitative differences to conventional semiconductors.

cond-mat.str-el

Chirped amplitude mode in photo-excited superconductors

Using a state-of-the-art numerical scheme, we show that the Higgs mode under excitation exhibits chirped oscillations and exponential decay when fluctuations are included. This is in stark contrast to conventional BCS collisionless dynamics which predict power-law decay and the absence of chirping. The chirped amplitude mode enables us to determine the local modification of the effective potential even when the system is in a long-lived prethermal state. We then show that this chirped amplitude mode is an experimentally observable quantity since the photoinduced (super)current in pump-probe experiments serves as an efficient proxy for the order parameter dynamics, including the chirped dynamics. Our result is based on the attractive Hubbard model using dynamical mean-field theory within the symmetry-broken state after a excitation across the superconducting gap. Since the collective response involves long timescales, we extend the hierarchical low-rank compression method for nonequilibrium Green's functions to symmetry-broken states and show that it serves as an efficient representation despite long-lived memory kernels.

cond-mat.supr-con

Bulk photovoltaic effect in antiferromagnet: Role of collective spin dynamics

Inspired by recent advancements in the bulk photovoltaic effect which can extend beyond the independent particle approximation (IPA), this study delves into the influence of collective spin dynamics in an antiferromagnetic on photocurrent generation using a time domain calculation. In the linear and photocurrent conductivity spectra, we observe peaks below the bandgap regime, attributed to the resonant contributions of collective modes, alongside broadband modifications resulting from off-resonant spin dynamics. Notably, the emergence of spin dynamics allows various types of photocurrent, which are absent in the IPA framework. Furthermore, we emphasize the importance of energy scale proximity between electronic and spin degrees of freedom in enabling efficient feedback between them. These findings offer new avenues for efficient energy harvesting and optoelectronic applications.

cond-mat.mtrl-sci

Dynamical exciton condensates in biased electron-hole bilayers

Bilayer materials may support interlayer excitons comprised of electrons in one layer and holes in the other. In experiments, a non-zero exciton density is typically sustained by a bias chemical potential, implemented either by optical pumping or by electrical contacts connected to the two layers. We show that if charge can tunnel between the layers, the chemical potential bias means that an exciton condensate is in the dynamical regime of ac Josephson effect. It has physical consequences such as tunneling currents and the ability to tune a condensate from bright (emitting coherent photons) to dark by experimental controlling knobs. If the system is placed in an optical cavity, coupling with cavity photons favors different dynamical states depending on the bias, realizing superradiant phases.

cond-mat.mes-hall

Efficient Control of High Harmonic Generation in Carbon Nanotubes using the Aharonov-Bohm Effect

We show that high-harmonic generation (HHG) in carbon nanotubes (CNTs) can be efficiently controlled using the Aharanov-Bohm (AB) effect. When a static magnetic field (B) is applied along the tube, electronic wave functions acquire complex phases along the circumferential direction (AB effect), which modifies the band structure. In particular, when the magnetic field is applied to metallic CNTs, which can be regarded as one-dimensional massless Dirac systems, realistic values of B lead to a nonzero gap in the THz regime. We demonstrate that such change from gapless to gapped Dirac systems drastically increases the HHG intensity in the THz regime. In the gapless Dirac system, the velocity of each electron never changes under the electric field, and thus there is no HHG. On the other hand, the gap opening activates both the interband and itraband currents, which strongly contribute to HHG. Our work demonstrates a unique way to manipulate HHG in nanotubes by tuning electronic wave functions using the magnetic field and the tube structure.

cond-mat.mes-hall

Exciton-spin interactions in antiferromagnetic charge-transfer insulators

We derive exciton-spin interactions from a microscopic correlated model that captures important aspects of the physics of charge-transfer (CT) insulators to address magnetism associated with exciton creation. We present a minimal model consisting of coupled clusters of transition metal d and ligand p orbitals that captures the essential features of the local atomic and electronic structure. First, we identify the lowest-energy state and optically allowed excited states within a cluster by applying the molecular orbital picture to the ligand p orbitals. Then, we derive the effective interactions between two clusters mediated by intercluster hoppings, which include exciton-spin couplings. The interplay of the correlations and the spatial structure of the CT exciton leads to strong magnetic exchange couplings with spatial anisotropy. Finally, we calculate an optical excitation spectrum in our effective model to obtain insights into magnetic sidebands optically observed in magnetic materials. We demonstrate that the spin-flip excitation due to the strongly enhanced local spin interactions around the exciton gives rise to the magnetic sidebands.

cond-mat.str-el

Photo-induced nonequilibrium states in Mott insulators

The study of nonequilibrium phenomena in interacting lattice systems can provide new perspectives on correlation effects, and information on metastable states of matter. Mott insulators are a promising class of systems for nonequilibrium studies, since they exhibit exotic phenomena and complex phase diagrams upon doping, and because a large Mott gap provides protection against fast thermalization and heating after photo-excitations. We can thus expect the emergence of interesting transient states and photo-induced phases in Mott systems. This review presents the current understanding of the mechanisms which control the time evolution of photo-doped charge carriers and the properties of photo-induced metastable states. We focus on recent theoretical progress, identify the relevant underlying concepts, and link them to experimental observations. The review starts with a general discussion of field-induced nonequilibrium setups and an overview of key experiments which revealed characteristic properties of photo-excited Mott states, proceeds with a compact overview of the theoretical tools which have been developed to investigate these strongly correlated nonequilibrium states, and then analyzes Mott insulators driven out of equilibrium by static electric fields, periodic fields, and short laser pulses. We also discuss the appearance of nonthermal electronic orders in photo-excited Mott systems, including nonthermal spin and orbital orders, $\eta$ pairing states, and novel types of excitonic orders.

cond-mat.str-el

Suppression of Heating by Multi-color Driving Protocols in Floquet Engineered Strongly Correlated Systems

Heating effects in Floquet engineered system are detrimental to the control of physical properties. In this work, we show that the heating of periodically driven strongly correlated systems can be suppressed by multi-color driving, i.e., by applying auxiliary excitations which interfere with the absorption processes from the main drive. We focus on the Mott insulating single-band Hubbard model and study the effects of multi-color driving with nonequilibrium dynamical mean-field theory. The main excitation is a periodic electric field with frequency $Ω$ smaller than the Mott gap, while for the auxiliary excitations, we consider additional electric fields and/or hopping modulations with a higher harmonic of $Ω$. To suppress the 3-photon absorption of the main excitation, which is a parity-odd process, we consider auxiliary electric-field excitations and a combination of electric-field excitations and hopping modulations. On the other hand, to suppress the 2-photon absorption, which is a parity-even process, we consider hopping modulations. The conditions for an efficient suppression of heating are well captured by the Floquet effective Hamiltonian derived with the high-frequency expansion in a rotating frame. As an application, we focus on the exchange couplings of the spins (pseudo-spins) in the repulsive (attractive) model, and demonstrate that the suppression of heating allows to realize and clearly observe a significant Floquet-induced change of the low energy physics.

cond-mat.str-el

Energy flow during relaxation in an electron-phonon system with multiple modes: A nonequilibrium Green's function study

We investigate an energy flow in an extended Holstein model describing electron systems coupled to hot-phonons and heat-bath phonons. To analyze the relaxation process after the photo-excitation of electrons, we employ the nonequilibrium dynamical mean-field theory (DMFT). We find the backward energy flow during the relaxation, where the direction of energy transfer between electrons and hot-phonons is reversed. To clarify the microscopic mechanism of the backward energy flow, we introduce the approximated energy flows, which are calculated with the gradient and quasiparticle approximations and are related to the nonequilibrium distribution functions. We compare these approximated energy flows with the full energy flows calculated from the nonequilibrium DMFT. We find that, in the weak electron-hot-phonon coupling regime, the full and approximated energy flows are almost the same, meaning that the relaxation dynamics can be correctly understood in terms of the nonequilibrium distribution functions. As the strength of the electron-hot-phonon coupling increases, the approximated energy flow fails to qualitatively reproduce the full energy flow. This indicates that the microscopic origin of the energy flow cannot be solely explained by the nonequilibrium distribution functions. By comparing the energy flows with different levels of approximation, we reveal the role of the gradient and quasiparticle approximations.

cond-mat.str-el