arXiv subjects

Denis Golez

Publications and source records attributed to Denis Golez.

At least 19 recordsLinked to original sources

arXiv2024

Measuring the ultrafast screening of $U$ in photo-excited charge-transfer insulators with time-resolved X-ray absorption spectroscopy

Recent seminal experiments have utilized time-resolved X-ray absorption spectroscopy (XAS) to investigate the ultrafast photo-induced renormalization of the electron interaction (''Hubbard $U$'') in Mott and charge transfer insulators. In this paper, we analyze the change of interactions due to dynamical screening as it is encoded in the XAS signal, using the non-equilibrium GW+EDMFT formalism. Our study shows that XAS is well-suited for measuring this change, but two aspects should be kept in mind if the screening processes are not substantially faster than the valence electron dynamics: (i) Screening in a photo-excited system can affect both the position and the lineshape of the absorption lines. (ii) In general, the effect cannot be captured by the modification of a single interaction parameter. Specifically, an estimate for $\Delta U$ extracted from the shift of the XAS lines does not necessarily describe the related shift of the the upper Hubbard band. We clarify these aspects using a minimal cluster model and the three-band Emery model for a charge transfer insulator.

cond-mat.str-el↗

arXiv2023

Photo-induced charge-transfer renormalization in NiO

Photo-doped states in strongly correlated charge transfer insulators are characterized by $d$-$d$ and $d$-$p$ interactions and the resulting intertwined dynamics of charge excitations and local multiplets. Here we use femtosecond x-ray absorption spectroscopy in combination with dynamical mean-field theory to disentangle these contributions in NiO. Upon resonant optical excitation across the charge transfer gap, the Ni $L_3$ and O $K$ absorption edges red-shift for $>10$ ps, associated with photo-induced changes in the screening environment. An additional signature below the Ni $L_3$ edge is identified for $<1$ ps, reflecting a transient nonthermal population of local many-body multiplets. We employ a nonthermal generalization of the multiplet ligand field theory to show that the feature originates from $d$-$d$ transitions. Overall, the photo-doped state differs significantly from a chemically doped state. Our results demonstrate the ability to reveal excitation pathways in correlated materials by x-ray spectroscopies, which is relevant for ultrafast materials design.

cond-mat.str-el↗

arXiv2022

Local interpretation of time-resolved X-ray absorption in Mott insulators: Insights from nonequilibrium dynamical mean-field theory

We present a formalism based on nonequilibrium dynamical mean field theory (DMFT) which allows to compute the time-resolved X-ray absorption spectrum (XAS) of photo-excited solids. By applying this formalism to the photo-doped half-filled and quarter-filled two-orbital Hubbard models in the Mott insulating regime we clarify how the time-resolved XAS signal reflects the nonequilibrium population of different local states. Apart from the missing broadening associated with continuum excitations, the atomic XAS spectrum computed with the nonthermal state populations provides a good approximation to the full nonequilibrium DMFT result. This suggest a route to combine the accurate DMFT description of nonequilibrum states of solids with cluster calculations of the XAS signal.

cond-mat.str-el↗

arXiv2021

Unveiling the underlying interactions in Ta2NiSe5 from photo-induced lifetime change

We present a generic procedure for quantifying the interplay of electronic and lattice degrees of freedom in photo-doped insulators through a comparative analysis of theoretical many-body simulations and time- and angle-resolved photoemission spectroscopy (TR-ARPES) of the transient response of the candidate excitonic insulator Ta2NiSe5. Our analysis demonstrates that the electron-electron interactions dominate the electron-phonon ones. In particular, a detailed analysis of the TRARPES spectrum enables a clear separation of the dominant broadening (electronic lifetime) effects from the much smaller bandgap renormalization. Theoretical calculations show that the observed strong spectral broadening arises from the electronic scattering of the photo-excited particle-hole pairs and cannot be accounted for in a model in which electron-phonon interactions are dominant. We demonstrate that the magnitude of the weaker subdominant bandgap renormalization sensitively depends on the distance from the semiconductor/semimetal transition in the high-temperature state, which could explain apparent contradictions between various TR-ARPES experiments. The analysis presented here indicates that electron-electron interactions play a vital role (although not necessarily the sole one) in stabilizing the insulating state.

cond-mat.str-el↗

arXiv2021

Photo-induced phase transition and associated time scales in the excitonic insulator Ta$_2$NiSe$_5$

We investigate the non-equilibrium electronic structure and characteristic time scales in a candidate excitonic insulator, Ta$_2$NiSe$_5$, using time- and angle-resolved photoemission spectroscopy with a temporal resolution of 50 fs. Following a strong photoexcitation, the band gap closes transiently within 100 fs, i.e., on a time scale faster than the typical lattice vibrational period. Furthermore, we find that the characteristic time associated with the rise of the photoemission intensity above the Fermi energy decreases with increasing excitation strength, while the relaxation time of the electron population towards equilibrium shows an opposite behaviour. We argue that these experimental observations can be consistently explained by an excitonic origin of the band gap in the material. The excitonic picture is supported by microscopic calculations based on the non-equilibrium Green's function formalism for an interacting two-band system. We interpret the speedup of the rise time with fluence in terms of an enhanced scattering probability between photo-excited electrons and excitons, leading to an initially faster decay of the order parameter. We show that the inclusion of electron-phonon coupling at a semi-classical level changes only the quantitative aspects of the proposed dynamics, while the qualitative features remain the same. The experimental observations and microscopic calculations allow us to develop a simple and intuitive phenomenological model that captures the main dynamics after photoexcitation in Ta$_2$NiSe$_5$.

cond-mat.str-el↗

arXiv2020

$η$--paired superconducting hidden phase in photodoped Mott insulators

We show that a metastable $η$--pairing superconducting phase can be induced by photodoping doublons and holes into a strongly repulsive fermionic Hubbard model. The doublon-hole condensate originates from an intrinsic doublon-hole exchange interaction and does not rely on the symmetry of the half-filled Hubbard model. It extends over a wide range of doublon densities and effective temperatures. Different non-equilibrium protocols to realize this state are proposed and numerically tested. We also study the optical conductivity in the superconducting phase, which exhibits ideal metallic behavior, i.e., a delta function at zero-frequency in the conductivity, in conjunction with a negative conductivity at large frequencies. These characteristic optical properties can provide a fingerprint of the $η$-pairing phase in pump-probe experiments.

cond-mat.str-el↗

arXiv2020

Nonlinear spectroscopy of collective modes in excitonic insulator

The nonlinear optical response of an excitonic insulator coupled to lattice degrees of freedom is shown to depend in strong and characteristic ways on whether the insulating behavior originates primarily from electron-electron or electron-lattice interactions. Linear response optical signatures of the massive phase mode and the amplitude (Higgs) mode are identified. Upon nonlinear excitation resonant to the phase mode, a new in-gap mode at twice the phase mode frequency is induced, leading to a huge second harmonic response. Excitation of in-gap phonon modes leads to different and much smaller effects. A Landau-Ginzburg theory analysis explain these different behavior and reveals that a parametric resonance of the strongly excited phase mode is the origin of the photo-induced mode in the electron-dominant case. The difference in the nonlinear optical response serve as a measure of the dominant mechanism of the ordered phase.

cond-mat.str-el↗

arXiv2020

Electromagnetic coupling in tight-binding models for strongly correlated light and matter

We discuss the construction of low-energy tight-binding Hamiltonians for condensed matter systems with a strong coupling to the quantum electromagnetic field. Such Hamiltonians can be obtained by projecting the continuum theory on a given set of Wannier orbitals. However, different representations of the continuum theory lead to different low-energy formulations, because different representations may entangle light and matter, transforming orbitals into light-matter hybrid states before the projection. In particular, a multi-center Power-Zienau-Woolley transformation yields a dipolar Hamiltonian which incorporates the light-matter coupling via both Peierls phases and a polarization density. We compare this dipolar gauge Hamiltonian and the straightforward Coulomb gauge Hamiltonian for a one-dimensional solid, to describe sub-cycle light-driven electronic motion in the semiclassical limit, and a coupling of the solid to a quantized cavity mode which renormalizes the band-structure into electron-polariton bands. Both descriptions yield the same result when many bands are taken into account, but the dipolar Hamiltonian is more accurate when the model is restricted to few electronic bands, while the Coulomb Hamiltonian requires fewer electromagnetic modes.

cond-mat.str-el↗

arXiv2020

Superconducting optical response of photodoped Mott insulators

Ultrafast laser pulses can redistribute charges in Mott insulators on extremely short time scales, leading to the fast generation of photocarriers. It has recently been demonstrated that these photocarriers can form a novel $η$--paired condensate at low temperatures, featuring a staggered superconducting pairing field. In this conference paper, we discuss the origin of the $η$--paired hidden phase and its optical response which may be detected in a pump-probe experiment. The hidden phase may be relevant for possible light-induced superconductivity in Mott insulators.

cond-mat.str-el↗

arXiv2019

Multi-band non-equilibrium GW+EDMFT formalism for correlated insulators

We study the dynamics of charge-transfer insulators after a photo-excitation using the three-band Emery model which is relevant for the description of cuprate superconductors. We provide a detailed derivation of the nonequilibrium extension of the multi-band GW+EDMFT formalism and the corresponding downfolding procedure. The Peierls construction of the electron-light coupling is generalized to the multi-band case resulting in a gauge invariant combination of the Peierls intra-band acceleration and dipolar intra-band transitions. We apply the formalism to the study of momentum-dependent (inverse) photo-emission spectra and optical conductivities. The time-resolved spectral function shows a strong renormalization of the charge-transfer gap and a substantial broadening of some of the bands. While the upper Hubbard band exhibits a momentum-dependent broadening, an almost rigid band shift is observed for the ligand bands. The inverse photo-emission spectrum reveals that the inclusion of the non-local and inter-band charge fluctuations lead to a very fast relaxation of holes into the lower Hubbard band. Consistent with the changes in the spectral function, the optical conductivity shows a renormalization of the charge-transfer gap, which is proportional to the photo-doping. The details of the photo-induced changes strongly depend on the dipolar matrix elements, which calls for an ab-initio determination of these parameters.

cond-mat.str-el↗

arXiv2019

Photo-enhanced excitonic correlations in a Mott insulator with nonlocal interactions

We investigate the effect of nonlocal interactions on the photo-doped Mott insulating state of the two-dimensional Hubbard model using a nonequilibrium generalization of the dynamical cluster approximation. In particular, we compare the situation where the excitonic states are lying within the continuum of doublon-holon excitations to a set-up where the excitons appear within the Mott gap. In the first case, the creation of nearest-neighbor doublon-holon pairs by excitations across the Mott gap results in enhanced excitonic correlations, but these excitons quickly decay into uncorrelated doublons and holons. In the second case, photo-excitation results in long-lived excitonic states. While in a low-temperature equilibrium state, excitonic features are usually not evident in single-particle observables such as the photoemission spectrum, we show that the photo-excited nonequilibrium system can exhibit in-gap states associated with the excitons. The comparison with exact-diagonalization results for small clusters allows us to identify the signatures of the excitons in the photo-emission spectrum.

cond-mat.str-el↗

arXiv2019

A unification of the Holstein polaron and dynamic disorder pictures of charge transport in organic semiconductors

We present a unified and nonperturbative method for calculating spectral and transport properties of Hamiltonians with simultaneous Holstein (diagonal) and Peierls (off-diagonal) electron-phonon coupling. Our approach is motivated by the separation of energy scales in semiconducting organic molecular cystals, in which electrons couple to high-frequency intramolecular Holstein modes and to low-frequency intermolecular Peierls modes. We treat Peierls modes as quasi-classical dynamic disorder, while Holstein modes are included with a Lang-Firsov polaron transformation and no narrow-band approximation. Our method reduces to the popular polaron picture due to Holstein coupling and the dynamic disorder picture due to Peierls coupling. We derive an expression for efficient numerical evaluation of the frequency-resolved optical conductivity based on the Kubo formula and obtain the DC mobility from its zero-frequency component. We also use our method to calculate the electron-addition Green's function corresponding to the inverse photoemission spectrum. For realistic parameters, temperature-dependent DC mobility is largely determined by the Peierls-induced dynamic disorder with minor quantitative corrections due to polaronic band-narrowing, and an activated regime is not observed at relevant temperatures. In contrast, for frequency-resolved observables, a quantum mechanical treatment of the Holstein coupling is qualitatively important for capturing the phonon replica satellite structure.

cond-mat.mtrl-sci↗

arXiv2019

Entropy-cooled nonequilibrium states of the Hubbard model

We show that the recently proposed cooling-by-doping mechanism allows to efficiently prepare interesting nonequilibrium states of the Hubbard model. Using nonequilibrium dynamical mean field theory and a particle-hole symmetric setup with dipolar excitations to full and empty bands we produce cold photo-doped Mott insulating states with a sharp Drude peak in the optical conductivity, a superconducting state in the repulsive Hubbard model with an inverted population, and $\eta$-paired states in systems with a large density of doublons and holons. The reshuffling of entropy into full and empty bands not only provides an efficient cooling mechanism, it also allows to overcome thermalization bottlenecks and slow dynamics that have been observed in systems cooled by the coupling to boson baths.

cond-mat.str-el↗

arXiv2018

A comparative study of nonequilibrium insulator-to-metal transitions in electron-phonon systems

We study equilibrium and nonequilibrium properties of electron-phonon systems described by the Hubbard-Holstein model using the dynamical mean-field theory. In equilibrium, we benchmark the results for impurity solvers based on the one-crossing approximation and slave-rotor approximation against non-perturbative numerical renormalization group reference data. We also examine how well the low energy properties of the electron-boson coupled systems can be reproduced by an effective static electron-electron interaction. The one-crossing and slave-rotor approximations are then used to simulate insulator-to-metal transitions induced by a sudden switch-on of the electron-phonon interaction. The slave-rotor results suggest the existence of a critical electron-phonon coupling above which the system is transiently trapped in a non-thermal metallic state with coherent quasiparticles. The same quench protocol in the one-crossing approximation results in a bad metallic state.

cond-mat.str-el↗

arXiv2017

Nonequilibrium GW+EDMFT: Antiscreening and inverted populations from nonlocal correlations

We study the dynamics of screening in photo-doped Mott insulators with long-ranged interactions using a nonequilibrium implementation of the $GW$ plus extended dynamical mean field theory ($GW$+EDMFT) formalism. Our study demonstrates that the complex interplay of the injected carriers with bosonic degrees of freedom (charge fluctuations) can result in long-lived transient states with properties that are distinctly different from those of thermal equilibrium states. Systems with strong nonlocal interactions are found to exhibit a self-sustained population inversion of the doublons and holes. This population inversion leads to low-energy antiscreening which can be detected in time-resolved electron-energy loss spectra.

cond-mat.str-el↗

arXiv2015

Dynamics of screening in photo-doped Mott insulators

We use a nonequilibrium implementation of extended dynamical mean field theory to study the effect of dynamical screening in photo-excited Mott insulators. The insertion of doublons and holes adds low-energy screening modes and leads to a reduction of the Mott gap. The coupling to low-energy bosonic modes further- more opens new relaxation channels and significantly speeds up the thermalization process. We also consider the effect of the energy distribution of the doped carriers on the screening.

cond-mat.str-el↗

arXiv2014

Unusual Two-stage Dynamics of the Spin-Lattice Polaron Formation

We follow the formation of a spin-lattice polaron after a quantum quench that simulates absorption of the pump{pulse in the time-resolved experiments. We discover a two-stage relaxation where spin and lattice degrees of freedom represent an integral part of the relaxation mechanism. In the first stage the kinetic energy of the spin-lattice polaron relaxes towards its ground state value while relaxation processes via spin and phonon degrees of freedom remain roughly independent. In the second, typically much longer stage, a subsequent energy transfer between lattice and spin degrees of freedom via the charge carrier emerges. The excess local spin energy radiates away via magnon excitations.

cond-mat.str-el↗

arXiv2013

Lifshitz phase transitions in the ferromagnetic regime of the Kondo lattice model

We establish the low-temperature phase diagrams of the spin-1/2 and spin-1 Kondo lattice models as a function of the conduction-band filling n and the exchange coupling strength J in the regime of ferromagnetic effective exchange interactions (n ~< 0.5). We show that both models have several distinct ferromagnetic phases separated by continuous Lifshitz transitions of the Fermi-pocket vanishing or emergence type: one of the phases has a true gap in the minority band (half metal), the others only a pseudogap. They can be experimentally distinguished by their magnetization curves; only the gapped phase exhibits magnetization rigidity. We find that, quite generically, ferromagnetism and Kondo screening coexist rather than compete, both in spin-1/2 and spin-1 models. We compute the Curie temperatures and establish a "ferromagnetic Doniach diagram" for both models.

cond-mat.str-el↗