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The exploration of ultrafast phenomena is a frontier of condensed matter research, where the interplay of theory, computation, and experiment is unveiling new opportunities for understanding and engineering quantum materials. With the advent of advanced experimental techniques and computational tools, it has become possible to probe and manipulate nonequilibrium processes at unprecedented temporal and spatial resolutions, providing insights into the dynamical behavior of matter under extreme conditions. These capabilities have the potential to revolutionize fields ranging from optoelectronics and quantum information to catalysis and energy storage. This Roadmap captures the collective progress and vision of leading researchers, addressing challenges and opportunities across key areas of ultrafast science. Contributions in this Roadmap span the development of ab initio methods for time-resolved spectroscopy, the dynamics of driven correlated systems, the engineering of materials in optical cavities, and the adoption of FAIR principles for data sharing and analysis. Together, these efforts highlight the interdisciplinary nature of ultrafast research and its reliance on cutting-edge methodologies, including quantum electrodynamical density-functional theory, correlated electronic structure methods, nonequilibrium Green's function approaches, quantum and ab initio simulations.

Time-resolved X-ray absorption can reveal the dynamical screening of the local Coulomb interaction in strongly correlated photo-excited materials. Here, we focus on the theoretical prediction of X-ray absorption in the presence of dynamical screening using the strong coupling expansion, i.e., an expansion around the isolated absorption site in terms of the retarded interaction. The evaluation of higher order diagrams is made numerically feasible by an approach based on the decomposition of the retarded interaction into complex exponentials. With this, we evaluate the strong coupling series to third order on an electron-boson model of Holstein type. We demonstrate that in relevant coupling regimes, even low orders of the strong coupling expansion can give a significant correction over the previously used lowest order approximation., Comment: Figure data attached (see 'Other Formats > Source')

Understanding light-induced hidden orders is relevant for nonequilibrium materials control and future ultrafast technologies. Hidden superconducting order, in particular, has been a focus of recent experimental and theoretical efforts. In this study, we investigate the stability of light-induced $\eta$ pairing. Using a memory truncated implementation of nonequilibrium dynamical mean field theory (DMFT) and entropy cooling techniques, we study the long-time dynamics of the photoinduced superconducting state. In the presence of coupling to a cold phonon bath, the photodoped system reaches a quasi-steady state, which can be sustained over a long period of time in large-gap Mott insulators. We show that this long-lived prethermalized state is well described by the nonequilibrium steady state implementation of DMFT.

The quench dynamics of systems exhibiting cooperative or almost competitive orders in equilibrium are explored using Ginzburg-Landau theory plus fluctuations. We show that when the renormalization of the free energy by fluctuations is taken into account, anisotropic stiffnesses and relaxation rates of the order parameters can lead to a stabilization of ordered states at transient free energy minima which are distinct from any (global or local) minima of the equilibrium free energy. This theory demonstrates that nonequilibrium fluctuations play a pivotal role in forming nonthermal orders. As nonthermal order and nonthermal fluctuations mutually stabilize each other over some time, this mechanism could be seen as a nonequilibrium variant of the order-by-disorder phenomenon. We discuss the relevance of these findings for systems with intertwined orders, such as high-temperature superconductors and the kagome metals, as well as for systems that show orbital ordering., Comment: 17 pages, 11 figures

We discuss the evaluation of the integrals for intermediate-order diagrams in the self-consistent strong-coupling expansion on the Keldysh contour using Tensor Cross Interpolation (TCI). TCI is used to factorize the nested parts of the integrand, allowing the integral to be computed as a recursion of convolution integrals, which are efficiently evaluated using the Fast Fourier Transform. The evaluation of diagrams where all vertices lie on one branch of the Keldysh contour resembles the structure of the imaginary-time formalism. For diagrams with time arguments on both contour branches, we find that it can be advantageous to parametrize the integrals in terms of physical time arguments with an additional sum over Keldysh indices. We benchmark the solution in relevant test cases, including the single impurity Anderson model and an exactly solvable electron-boson model. While the bond dimension increases with diagram order, the TCI-based integration efficiently handles low-order diagrams, making it a promising approach to go beyond the non-crossing approximation in steady-state non-equilibrium dynamical mean-field theory simulations., Comment: 18 pages, 13 figures

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.

Recent experiments demonstrate precise control over coherently excited circular phonon modes using high-intensity terahertz lasers, opening new pathways towards dynamical, ultrafast design of magnetism in functional materials. While the phonon Zeeman effect enables a theoretical description of phonon-induced magnetism, it lacks efficient angular momentum transfer from the phonon to the electron sector. In this work, we put forward a coupling mechanism based on electron-nuclear quantum geometry, with the inverse Faraday effect as a limiting case. This effect is rooted in the phase accumulation of the electronic wavefunction under a circular evolution of nuclear coordinates. An excitation pulse then induces a transient level splitting between electronic orbitals that carry angular momentum. First-principle simulations on SrTiO$_3$ demonstrate that in parts of the Brillouin zone, this splitting between orbitals carrying angular momentum can easily reach 50 meV., Comment: 6 pages, 3 figures, supplementary information, accepted in PRL

Cavity electrodynamics is emerging as a promising tool to control chemical processes and quantum material properties. In this work we develop a formalism to describe the cavity mediated energy exchange between a material and its electromagnetic environment. We show that coplanar cavities can significantly affect the heat load on the sample if the cavity resonance lies within the frequency region where free-space radiative heat dominates, typically the mid-IR at ambient temperature, while spectral filtering is necessary for having an effect with lower frequency cavities.

When light and matter interact strongly, the coupled system inherits properties from both constituents. It is consequently possible to alter the properties of either by engineering the other. This intriguing possibility has lead to the emergence of the cavity-materials-engineering paradigm which seeks to tailor material properties by engineering the fluctuations of a dark electromagnetic environment. The theoretical description of hybrid light-matter systems is complicated by the combined complexity of a realistic description of the extended electronic and quantum electromagnetic fields. Here we derive an effective, non-perturbative theory for low dimensional crystals embedded in a paradigmatic Fabry-P\'erot resonator in the long-wavelength limit. The theory encodes the multi-mode nature of the electromagnetic field into an effective single-mode scheme and it naturally follows from requiring a negligible momentum transfer from the photonic system to the matter. Crucially, in the effective theory the single light mode is characterized by a finite effective mode volume even in the limit of bulk cavity-matter systems and can be directly determined by realistic cavity parameters. As a consequence, the coupling of the effective mode to matter remains finite for bulk materials. By leveraging on the realistic description of the cavity system we make our effective theory free from the double counting of the coupling of matter to the electromagnetic vacuum fluctuations of free space. Our results provide a substantial step towards the realistic description of interacting cavity-matter systems at the level of the fundamental Hamiltonian, by effectively including the electromagnetic environment and going beyond the perfect mirrors approximation.

A description of long-lived photo-doped states in Mott insulators is challenging, as it needs to address exponentially separated timescales. We demonstrate how properties of such states can be computed using numerically exact steady state techniques, in particular Quantum Monte Carlo, by using a time-local ansatz for the distribution function with separate Fermi functions for the electron and hole quasiparticles. The simulations show that the Mott gap remains robust to large photo-doping, and the photo-doped state has hole and electron quasiparticles with strongly renormalized properties., Comment: 9 pages, 9 figures

We investigate the potential to induce long-range spin interactions in a Mott insulator via the quantum electromagnetic field of a cavity. The coupling between light and spins is inherently non-linear, and occurs via multi-photon processes like Raman scattering and two-photon absorption/emission with electronically excited intermediate states. Based on this, two pathways are elucidated: (i) In the absence of external driving, long-range interactions are mediated by the exchange of at least two virtual cavity photons. We show that these vacuum-mediated interactions can surpass local Heisenberg interactions in mesoscopic setups such as sufficiently small split-ring resonators. (ii) In a laser-driven cavity, interactions can be tailored through a hybrid scheme involving both external laser photons and cavity photons. This offers a versatile pathway for Floquet engineering of long-range interactions in macroscopic systems. In general, the derivation of these interactions requires careful consideration: Notably, we demonstrate that a simple phenomenological approach, based on a spin-photon Hamiltonian that captures Raman and two-photon processes with effective matrix elements, can be used only if the cavity is resonantly driven. Outside of these narrow resonant regimes as well as for the undriven case, a fourth-order series expansion within the underlying electronic model is necessary, which we perform to obtain long-range four-spin interactions in the half-filled Hubbard model., Comment: 25 pages, 9 figures

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., Comment: Review article

Raman spectroscopy uses light scattering to extract information on low-energy excitations of solids. The Raman process is described by diagrams which are fourth order in the light-matter interaction, and in particular the resonant contribution, which involves four different space-time arguments, is difficult to evaluate. If one instead simulates explicitly the incoming (classical) light pulse, the Raman signal is given by the outgoing photon flux and can be determined from a two-point correlation function. Such a formalism can be used to compute the time-resolved Raman spectrum of non-equilibrium systems, as well as nonlinear signals which are higher order in the incoming field, such as hyper Raman scattering. Here we explain how to implement this time-dependent formalism within the dynamical mean field theory framework. The method is illustrated with applications to the Holstein-Hubbard model in the strong electron-phonon coupling regime. We demonstrate hyper Raman scattering in measurements with strong probe fields and frequency mixing signals in the presence of a pump field, and simulate the evolution of Stokes and anti-Stokes features after photo-excitations of metallic and Mott insulating systems.

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.

Sr$_2$IrO$_4$ has attracted a lot of attention due to its structural and electronic similarities to La$_2$CuO$_4$ which is the parent compound of high-T$_c$ superconducting cuprates. It was proposed to be a strong spin-orbit coupled J$_{eff}$ = 1/2 Mott insulator, but the Mott nature of its insulating ground state and the origin of the gap have not been conclusively established. Here, we use ultrafast laser pulses to realize an insulator-metal transition in Sr$_2$IrO$_4$ and probe the resulting dynamics using time- and angle-resolved photoemission spectroscopy. We observe a closing of the gap and the formation of weakly-renormalized electronic bands in the gap region. Comparing these observations to the expected temperature and doping evolution of Mott gaps and Hubbard bands provides clear evidence that the insulating state does not originate from Mott correlations. We instead propose a correlated band insulator picture, where antiferromagnetic correlations play a key role in the opening of the gap. More broadly, our results demonstrate that energy-momentum resolved nonequilibrium dynamics can be used to clarify the nature of equilibrium states in correlated materials.

Recent theoretical studies showed that the electronic structure of 1$T$-TaS$_2$ in the low-temperature commensurate charge density wave phase exhibits a nontrivial interplay between band-insulating and Mott insulating behavior. This has important implications for the interpretation of photo-doping experiments. Here we use nonequilibrium dynamical mean-field theory simulations of a realistic multi-layer structure to clarify the charge carrier dynamics induced by a laser pulse. The solution is propagated up to the picosecond timescale by employing a memory-truncation scheme. While long-lived doublons and holons only exist in the surface state of a specific structure, the disturbance of bonding states in the bilayers which make up the bulk of the system explain the almost instantaneous appearance of in-gap states. Our simulations consistently explain the coexistence of a doublon feature with a prominent ``background" signal in previous time-resolved photoemission experiments, and they suggest strategies for the selective population of the ingap and doublon states by exploiting the sensitivity to the pump polarization and pump frequency., Comment: 12 pages, 9 figures

Placing quantum materials into optical cavities provides a unique platform for controlling quantum cooperative properties of matter, via both weak and strong light-matter coupling. Here we report the experimental evidence of reversible cavity control of a metal-to-insulator phase transition in a correlated solid-state material. We embed the charge density wave material 1T-TaS$_{2}$ into cryogenic tunable terahertz cavities and show that a switch between conductive and insulating behaviors, associated with a large change in the sample temperature, is obtained by mechanically tuning the distance between the cavity mirrors and their alignment. The large thermal modification observed is indicative of a Purcell-like scenario in which the spectral profile of the cavity modifies the energy exchange between the material and the external electromagnetic field. Our findings provide opportunities for controlling the thermodynamics and macroscopic transport properties of quantum materials by engineering their electromagnetic environment., Comment: 52 pages, 36 figures (including Supplementary Information)

Inspired by the physics of rare earth nickelates, we study the photoemission (PES) and resonant inelastic X-ray scattering (RIXS) spectra of a correlated electron system with two types of insulating sublattices. Sublattice A is characterized by a hybridization gap and a low-spin state, while sublattice B features a Mott gap and a local magnetic moment. We show how the coupling of these two qualitatively different insulating states affects the dynamics of photo-induced charge carriers and how the nonequilibrium states manifest themselves in the PES and RIXS signals. In particular, we find that charge carriers created on the B sublattice migrate to the A sublattice, where they contribute to the creation of in-gap states in the PES signal, and to characteristic peaks in the nonequilibrium RIXS spectrum. While the contributions from the two sublattices cannot be easily distinguished in the local photoemission spectrum, the weights of the RIXS signals in the two-dimensional $\omega_\text{in}$-$\omega_\text{out}$ space provide information on the local state evolution on both sublattices.

The interplay of light and matter gives rise to intriguing cooperative effects in quantum many-body systems. This is even true in thermal equilibrium, where the electromagnetic field can hybridize with collective modes of matter, and virtual photons can induce interactions in the solid. Here, we show how these light-mediated interactions can be treated using the dynamical mean-field theory formalism. We consider a minimal model of a two-dimensional material that couples to a surface plasmon polariton mode of a metal-dielectric interface. Within the mean-field approximation, the system exhibits a ferroelectric phase transition that is unaffected by the light-matter coupling. Bosonic dynamical mean-field theory provides a more accurate description and reveals that the photon-mediated interactions enhance the ferroelectric order and stabilize the ferroelectric phase.

We discuss a semiclassical approach to solve the quantum impurity model within non-equilibrium dynamical mean-field theory for electron-lattice models. The effect of electronic fluctuations on the phonon is kept beyond Ehrenfest dynamics, leading to a stochastic phonon evolution with damping and noise terms that are self-consistently determined by the electronic correlation functions in the fluctuating phonon field. Together with a solution of the electronic model based on a non-perturbative quantum Boltzmann equation, the approach can be used to address the coupled dynamics of the electrons and the lattice during photo-induced phase transitions. Results for the Anderson-Holstein model are benchmarked against numerically exact quantum Monte Carlo data. We find good agreement for the phonon distribution function at temperatures comparable to the charge ordering temperature. The general formulation can be extended to models with electron-electron interactions or multi-orbital systems., Comment: 17 pages, 4 figures

We investigate the impact of a bosonic degree of freedom on Yu-Shiba-Rusinov (YSR) states emerging from a magnetic impurity in a conventional superconductor. Starting from the Anderson impurity model, we predict that an additional p-wave conduction band channel opens up if a bosonic mode is coupled to the tunnelling between impurity and host, which implies an additional pair of odd-parity YSR states. The bosonic mode can be a vibrational mode or the electromagnetic field in a cavity. The exchange couplings in the two channels depend sensitively on the state of the bosonic mode (ground state, few quanta or classically driven Floquet state), which opens possibilities for phononics or photonics control of such systems, with a rich variety of ground and excited states.

We investigate the control of interacting matter through strong coupling to a single electromagnetic mode, such as the photon mode in a Fabry-Perot or split-ring cavity. For this purpose, we analyze the exact effective theory for the collective light-matter hybrid modes of a generic system of $N$ transition dipoles within an interacting solid. The approach allows to predict properties of the coupled light-matter system from the nonlinear response functions of the uncoupled matter ``outside the cavity''. The limit of large $N$ corresponds to a conventional macroscopic description based on the polarizability of matter. In this limit, the cavity does not affect the static ferroelectric response. Corrections, which are needed to understand finite size systems and to obtain the nonlinear light-matter response, can be obtained from the non-linear susceptibilities of the matter outside the cavity. The theory is benchmarked for the Dicke model, and for a quantum Ising model which serves as a minimal mean-field model for a quantum paraelectric material like SrTiO3., Comment: 20 pages, 6 figures

We present a quantum impurity solver based on a pseudo-particle framework, which combines diagrammatic resummations for a three-point vertex with diagrammatic Monte Carlo sampling of a four-point vertex. This recently proposed approach [A. J. Kim et al., arXiv:2112.15549] is generalized here to fermionic impurity problems and we discuss the technical details of the implementation, including the time-stepping approach, the Monte Carlo updates, and the routines for checking the two-particle irreducibility of the four-point vertex. We also explain how the vertex information can be efficiently stored using a Dubiner basis representation. The convergence properties of the algorithm are demonstrated with applications to exactly solvable impurity models and dynamical mean field theory simulations of the single-orbital Hubbard model. It is furthermore shown that the algorithm can handle a two-orbital problem with off-diagonal hybridizations, which would cause a severe sign problem in standard hybridization-expansion Monte Carlo simulations. Since the vertex-based algorithm successfully handles sign oscillating integrals in equilibrium and samples only connected diagrams, it may be a promising approach for real-time simulations., Comment: 16 pages, 21 figures

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.

We overview the concept of dynamical phase transitions in isolated quantum systems quenched out of equilibrium. We focus on non-equilibrium transitions characterized by an order parameter, which features qualitatively distinct temporal behaviour on the two sides of a certain dynamical critical point. Dynamical phase transitions are currently mostly understood as long-lived prethermal phenomena in a regime where inelastic collisions are incapable to thermalize the system. The latter enables the dynamics to substain phases that explicitly break detailed balance and therefore cannot be encompassed by traditional thermodynamics. Our presentation covers both cold atoms as well as condensed matter systems. We revisit a broad plethora of platforms exhibiting pre-thermal DPTs, which become theoretically tractable in a certain limit, such as for a large number of particles, large number of order parameter components, or large spatial dimension. The systems we explore include, among others, quantum magnets with collective interactions, $\phi^4$ quantum field theories, and Fermi-Hubbard models. A section dedicated to experimental explorations of DPTs in condensed matter and AMO systems connects this large variety of theoretical models., Comment: 37 pages; 10 figures; review article

We propose a diagrammatic Monte Carlo approach for general spin-boson models, which can be regarded as a generalization of the strong-coupling expansion for fermionic impurity models. The algorithm is based on a self-consistently computed three-point vertex and a stochastically sampled four-point vertex, and achieves convergence to the numerically exact result in a wide parameter regime. The performance of the algorithm is demonstrated with applications to a spin-boson model representing an emitter in a waveguide. As a function of the coupling strength, the spin exhibits a delocalization-localization crossover at low temperatures, signaling a qualitative change in the real-time relaxation. In certain parameter regimes, the response functions of the emitter coupled to the electromagnetic continuum can be described by an effective Rabi model with appropriately defined parameters. We also discuss the spatial distribution of the photon density around the emitter., Comment: 11 pages, 7 figures

Using ultrashort laser pulses, it has become possible to probe the dynamics of long-range order in solids on microscopic timescales. In the conventional description of symmetry-broken phases within time-dependent Ginzburg-Landau theory, the order parameter evolves coherently, with small fluctuations along an average trajectory. Recent experiments, however, indicate that some systems can support a different scenario, named ultrafast inhomogeneous disordering, where the average order parameter is no longer representative of the state on the atomic scale. Here we theoretically show that ultrafast disordering can occur in a minimal, yet paradigmatic, model for a Peierls instability if atomic scale inhomogeneities of both the electronic structure and the charge density wave order parameter are taken into account. The latter is achieved using a non-equilibrium generalization of statistical dynamical mean-field theory, coupled to stochastic differential equations for the order parameter., Comment: 13 pages, 7 figures

The Keldysh formalism for nonequilibrium Green's functions is a powerful theoretical framework for the description of the electronic structure, spectroscopy, and dynamics of strongly correlated systems. However, the underlying Kadanoff-Baym equations (KBE) for the two-time Keldysh Green's functions involve a memory kernel which results in a high computational cost for long simulation times $t_\text{max}$, with a cubic scaling of the computation time with $t_\text{max}$. Truncation of the memory kernel can reduce the computational cost to linear scaling with $t_\text{max}$, but the required memory times will depend on the model and the diagrammatic approximation to the self-energy. We explain how a truncation of the memory kernel can be incorporated into the time-propagation algorithm to solve the KBE, and investigate the systematic truncation of the memory kernel for the Hubbard model in different parameter regimes, and for different diagrammatic approximations. The truncation is easier to control within dynamical mean-field solutions, where it is applied to a momentum-independent self-energy. Here, simulation times up to two orders of magnitude longer are accessible both in the weak and strong coupling regime, allowing for a study of long-time phenomena such as the crossover between pre-thermalization and thermalization dynamics., Comment: 14 pages, 11 figures

Quasi-one-dimensional systems exhibit many-body effects elusive in higher dimensions. A prime example is spin-orbital separation, which has been measured by resonant inelastic X-ray scattering (RIXS) in Sr$_2$CuO$_3$. Here, we theoretically analyze the time-resolved RIXS spectrum of Sr$_2$CuO$_3$ under the action of a time-dependent electric field. We show that the external field can reversibly modify the parameters in the effective $t-J$ model used to describe spinon and orbiton dynamics in the material. For strong driving amplitudes, we find that the spectrum changes qualitatively as a result of reversing the relative spinon to orbiton velocity. The analysis shows that in general, the spin-orbital dynamics in Mott insulators in combination with time-resolved RIXS should provide a suitable platform to explore the reversible control of many-body physics in the solid with strong laser fields., Comment: 13 pages, 4 figures

The optical conductivity contains information about energy absorption and the underlying physical processes. In finite-dimensional systems, vertex corrections to the bare bubble need to be considered, which is a computationally challenging task. Recent numerical studies showed that in the weak coupling limit, near an ordering instability with wave vector $\pi$, $\pi$-tons (or Maki-Thompson diagrams) yield the most relevant vertex corrections. This provides a route for including vertex corrections into, for example, dynamical mean field theory estimates of the optical conductivity. By implementing calculations on the Kadanoff-Baym contour, we reveal the characteristic spectral signatures of the $\pi$-tons and their evolution under non-equilibrium conditions. We consider interaction quenches of the weakly-correlated Hubbard model near the antiferromagnetic phase boundary, and analyze the evolution of the Drude and $\pi$-ton features. While the bubble contribution to the optical conductivity is found to thermalize rapidly, after some oscillations with frequencies related to the local spectral function, the $\pi$-ton contribution exhibits a slower evolution. We link this observation to the prethermalization phenomenon which has been previously studied in weakly interacting, quenched Hubbard models., Comment: 15 pages, 12 figures

Recent experiments have revealed the tantalizing possibility of fabricating lattice electronic systems strongly coupled to quantum fluctuations of electromagnetic fields, e.g., by means of geometry confinement from a cavity or artificial gauge fields in quantum simulators. In this work, we develop a high-frequency expansion to construct the effective models for lattice electrons strongly coupled to a continuum of off-resonant photon modes with arbitrary dispersion. The theory is nonperturbative in the light-matter coupling strength, and is therefore particularly suitable for the ultrastrong light-matter coupling regime. Using the effective models, we demonstrate how the dispersion and topology of the electronic energy bands can be tuned by the cavity. In particular, quasi-one-dimensional physics can emerge in a two-dimensional square lattice due to a spatially anisotropic band renormalization, and a topologically nontrivial anomalous quantum Hall state can be induced in a honeycomb lattice when the cavity setup breaks time-reversal symmetry. We also demonstrate that the photon-mediated interaction induces an unconventional superconducting paired phase distinct from the pair-density-wave state discussed in models with truncated light-matter coupling. Finally, we study a realistic setup of a Fabry-P\'{e}rot cavity. Our work provides a systematic framework to explore the emergent phenomena due to strong light-matter coupling and points out new directions of engineering orders and topological states in solids.

We use the nonequilibrium dynamical mean field theory formalism to compute the equilibrium and nonequilibrium resonant inelastic X-ray scattering (RIXS) signal of a strongly interacting fermionic lattice model with a coupling of dispersionless phonons to the total charge on a given site. In the atomic limit, this model produces phonon subbands in the spectral function, but not in the RIXS signal. Electron hopping processes however result in phonon-related modifications of the charge excitation peak. We discuss the equilibrium RIXS spectra and the characteristic features of nonequilibrium states induced by photo-doping and by the application of a static electric field. The latter produces features related to Wannier-Stark states, which are dressed with phonon sidebands. Thanks to the effect of field-induced localization, the phonon features can be clearly resolved even in systems with weak electron-phonon coupling.

Light-manipulation of correlated electronic phases in solids offers the tantalizing prospect of realizing electronic devices operating at the ultrafast time-scale. In this context, the experimental realization of non-equilibrium transitions from a metal to a band or Mott insulator has shown to be particularly elusive. Using dynamical mean-field theory, we study a simple model representing the main physical properties of the oxygen-enriched compound LaTiO$_{3+x}$. By properly optimizing the photo-doping of electrons from a low-energy band into the valence states of the system, we show it is possible to induce a valence transition from a correlated metallic state to a Mott insulator at ultrashort time scales and to contain the heating during this process, with the final non-thermal valence insulator having almost the same effective temperature of the starting metal., Comment: 9 pages, 7 figures

Orbitally ordered states exhibit unique features which make them a promising platform for exploring the ultrafast dynamics of long-range order in solids: Their free energy typically has multiple discrete minima, and electric laser fields or selectively excited phonons can exert effective forces that may be used to steer the order parameter through these free energy landscapes. Moreover, their free energy strongly depends on fluctuations, and in some cases restoring forces close to a minimum are exclusively of entropic origin (order-by-disorder mechanisms). This can open pathways to control the dynamics of the order parameter via non-thermal fluctuations. In this work, we study the laser-induced non-equilibrium dynamics in a $120^\circ$ compass model, using time-dependent Ginzburg-Landau theory. We analyze protocols to switch the order parameter between equivalent configurations, with a focus on the interplay between the external force due to the driving field, and the non-thermal entropic forces. In particular, we find that remanent non-thermal fluctuations after some excitation can stabilize the high-symmetry phase even when the homogeneous potential has retrieved its low-temperature form, which facilitates laser-induced switching., Comment: 12 pages, 8 figures

Collective orders and photo-induced phase transitions in quantum matter can evolve on timescales which are orders of magnitude slower than the femtosecond processes related to electronic motion in the solid. Quantum Boltzmann equations can potentially resolve this separation of timescales, but are often constructed within a perturbative framework. Here we derive a quantum Boltzmann equation which only assumes a separation of timescales (taken into account through the gradient approximation for convolutions in time), but is based on a non-perturbative scattering integral, and makes no assumption on the spectral function such as the quasiparticle approximation. In particular, a scattering integral corresponding to non-equilibrium dynamical mean-field theory is evaluated in terms of an Anderson impurity model in a non-equilibrium steady state with prescribed distribution functions. This opens the possibility to investigate dynamical processes in correlated solids with quantum impurity solvers designed for the study of non-equilibrium steady states., Comment: 11 pages, 3 figures

Resonant inelastic X-ray scattering (RIXS) detects various types of high- and low-energy elementary excitations in correlated solids, and this tool will play an increasingly important role in investigations of time-dependent phenomena in photo-excited systems. While theoretical frameworks for the computation of equilibrium RIXS spectra are well established, the development of appropriate methods for nonequilibrium simulations are an active research field. Here, we apply a recently developed nonequilibrium dynamical mean field theory (DMFT) based approach to compute the RIXS response of photo-excited two-orbital Mott insulators. The results demonstrate the feasibility of multi-orbital nonequilibrium RIXS calculations and the sensitivity of the quasi-elastic fluorescence-like features and d-d excitation peaks on the nonequilibrium population of the Hubbard bands.

We develop a framework to evaluate the time-dependent resonant inelastic X-ray scattering (RIXS) signal with the use of non-equilibrium dynamical mean field theory simulations. The approach is based on the solution of a time-dependent impurity model which explicitly incorporates the probe pulse. It avoids the need to compute four-point correlation functions, and can in principle be combined with different impurity solvers. This opens a path to study time-resolved RIXS processes in multi-orbital systems. The approach is exemplified with a study of the RIXS signal of a melting Mott antiferromagnet., Comment: 11 pages, 6 figures

We study the photoinduced ultrafast dynamics in relativistic Mott insulators, i.e., Mott insulators with strong spin-orbit coupling. For this purpose, we consider a minimal one-band Hubbard model on lattices with square and triangular symmetries, as relevant for layered transition metal compounds such as Sr$_2$IrO$_4$. Depending on the lattice and the spin-orbit coupling, the systems have canted antiferromagnetic or $120^\circ$ order. They are excited by simulating a short laser pulse, and the dynamics is solved using nonequilibrium dynamical mean-field theory. The pulse generates hot carriers, which subsequently perturb the magnetic order due to the coupling between the collective order and photocarriers. We find that this dynamics, which is known form regular antiferromagnets, depends sensitively on the spatial structure of the spin-orbit coupling. On the triangular lattice, in particular, relaxation times are influenced by the spin-orbit coupling for the chiral $120^\circ$ order, while on the square lattice with canted antiferromagnetic order the spin-orbit induced canting angle remains unchanged after the excitation. Our study opens up new possibilities of controlling magnetism and exotic spin states on the ultrafast timescales., Comment: 10 pages, 6 figures

Photo-doping of Mott insulators or correlated metals can create an unusual metallic state which simultaneously hosts hole-like and electron-like particles. We study the dynamics of this state up to long times, as it passes its kinetic energy to the environment. When the system cools down, it crosses over from a bad metal into a resilient quasiparticle regime, in which quasiparticle bands are formed with separate Fermi levels for electrons and holes, but quasiparticles do not yet satisfy the Fermi liquid paradigm. Subsequently, the transfer of energy to the environment slows down significantly, and the system does not reach the Fermi liquid state even on the timescale of picoseconds. The transient photo-doped strange metal exhibits unusual properties of relevance for ultrafast charge and heat transport: In particular, there can be an asymmetry in the properties of electrons and holes, and strong correlations between electrons and holes, as seen in the spectral properties., Comment: 7 pages, 6 figures

We study the melting of long-range antiferromagnetic order in the Hubbard model after an interaction quench, using non-equilibrium dynamical mean-field theory. From previous studies, the system is known to quickly relax into a prethermal symmetry-broken state. Using a convergent truncation of the memory integrals in the Kadanoff Baym equations, we unravel the subsequent relaxation dynamics of this state over several orders of magnitude in time. At long times, the prethermal state can be characterized by a single slow variable which is related to the conduction band population. The dynamics of this variable does not follow the paradigmatic steady relaxation of pre-thermal states: It is highly nonlinear, with a pronounced speedup once the gap falls below a certain value. This behavior indicates that non-thermal order can be self-stabilized on some timescale. It is not reproduced using simple Fermi's golden rule estimate for the evolution of the conduction band population., Comment: 11 pages, 5 figures

Photodoped states are widely observed in laser-excited Mott insulators, in which charge excitations are quickly created and can exist beyond the duration of the external driving. Despite the fruitful experimental explorations, theoretical studies on the microscopic models face the challenge to simultaneously deal with exponentially separated time scales, especially in multi-band systems, where the long-time behaviors are often well beyond the reach of state-of-the-art numerical tools. Here, we address this difficulty by introducing a steady-state description of photodoped Mott insulators using an open-system setup, where the photodoped system is stabilized as a non-equilirium steady-state (NESS) by a weak external driving. Taking advantage of the stationarity, we implement and discuss the details of an efficient numerical tool using the steady-state Dynamical Mean-Field Theory (DMFT), combined with the non-crossing approximation (NCA). We demonstrate that these stationary photodoped states exhibit the same properties of their transient counterparts, while being solvable with reasonable computational efforts. Furthermore, they can be parametrized by just few physical quantities, including the effective temperature and the density of charge excitations, which confirms the universal nature of photodoped states indeed independent of the excitation protocols. As a first application, we consider the stationary photodoped states in a two-band Hubbard model with intertwined spin-and-orbital ordering and find a family of hidden phases unknown from the previous studies, implying an apparently unexplored time regime of the relaxation of the intertwined orders.

We investigate the dynamics of superconducting fluctuations in the attractive three-dimensional Hubbard model after a quench from the disordered phase to the ordered regime. While the long time evolution is well understood in terms of dissipative time-dependent Ginzburg-Landau models with unstable potentials, early times are more demanding due to the inseparable dynamics of the pairing fluctuations and the electronic quasiparticles. Our simulation using the time-dependent fluctuation exchange approximation treat both degrees of freedom on the same footing and reveal a non-thermal electronic regime causing a non-monotonous growth of the fluctuations. This feature is not directly captured from the Ginzburg-Landau theory, but nevertheless remains observable beyond the thermalization time of the electrons. We further explore how the growth of the order parameter fluctuations leads to an opening of a pseudo-gap in the electronic spectrum, and identify Andreev reflections as the dominant mechanism behind the gap opening., Comment: 8 pages, 7 figures

We investigate out-of-equilibrium dynamics in an excitonic insulator (EI) with a finite momentum pairing perturbed by a laser-pulse excitation and a sudden coupling to fermionic baths. The transient dynamics of the excitonic order parameter is resolved using the full nonequilibrium Green's function approach and the generalized Kadanoff-Baym ansatz (GKBA) within the second-Born approximation. The comparison between the two approaches after a laser pulse excitation shows a good agreement in the weak and the intermediate photo-doping regime. In contrast, the laser-pulse dynamics resolved by the GKBA does not show a complete melting of the excitonic order after a strong excitation. Instead we observe persistent oscillations of the excitonic order parameter with a predominant frequency given by the renormalized equilibrium bandgap. This anomalous behavior can be overcome within the GKBA formalism by coupling to an external bath, which leads to a transition of the EI system towards the normal state. We analyze the long-time evolution of the system and distinguish decay timescales related to dephasing and thermalization., Comment: 13 pages, 12 figures

Nonlinear phononics holds the promise for controlling properties of quantum materials on the ultrashort timescale. Using nonequilibrium dynamical mean-field theory, we solve a model for the description of organic solids, where correlated electrons couple nonlinearly to a quantum phonon mode. Unlike previous works, we exactly diagonalize the local phonon mode within the noncrossing approximation to include the full phononic fluctuations. By exciting the local phonon in a broad range of frequencies near resonance with an ultrashort pulse, we show it is possible to induce a Mott insulator-to-metal phase transition. Conventional semiclassical and mean-field calculations, where the electron-phonon interaction decouples, underestimate the onset of the quasiparticle peak. This fact, together with the nonthermal character of the photoinduced metal, suggests a leading role of the phononic fluctuations and of the dynamic nature of the state in the vibrationally induced quasiparticle coherence.

We theoretically investigate the effects of the lattice geometry on the nonequilibrium dynamics of photo-excited carriers in a half-filled two-dimensional Hubbard model. Using a nonequilibrium generalization of the dynamical cluster approximation, we compare the relaxation dynamics in lattices which interpolate between the triangular lattice and square lattice configuration and thus reveal the role of the geometric frustration in these strongly correlated nonequilibrium systems. In particular, we show that the cooling effect resulting from the disordering of the spin background is less effective in the triangular case because of the frustration. This manifests itself in a longer relaxation time of the photo-doped population, as measured by the time-resolved photo-emission signal, and a higher effective temperature of the photo-doped carriers in the non-thermal steady state after the intra-Hubbard-band thermalization., Comment: 10 pages, 5 figures

Intertwined orders exist ubiquitously in strongly correlated electronic systems and lead to intriguing phenomena in quantum materials. In this paper, we explore the unique opportunity of manipulating intertwined orders through entangling electronic states with quantum light. Using a quantum Floquet formalism to study the cavity-mediated interaction, we show the vacuum fluctuations effectively enhance the charge-density-wave correlation, giving rise to a phase with entangled electronic order and photon coherence, with putative superradiant behaviors in the thermodynamic limit. Furthermore, upon injecting even one single photon in the cavity, different orders, including $s$--wave and $\eta$--paired superconductivity, can be selectively enhanced. Our study suggests a new and generalisable pathway to control intertwined orders and create light-matter entanglement in quantum materials. The mechanism and methodology can be readily generalised to more complicated scenarios., Comment: 6 pages + appendix

Light-matter coupling involving classical and quantum light offers a wide range of possibilities to tune the electronic properties of correlated quantum materials. Two paradigmatic results are the dynamical localization of electrons and the ultrafast control of spin dynamics, which have been discussed within classical Floquet engineering and in the deep quantum regime where vacuum fluctuations modify the properties of materials. Here we discuss how these two extreme limits are interpolated by a cavity which is driven to the excited states. In particular, this is achieved by formulating a Schrieffer-Wolff transformation for the cavity-coupled system, which is mathematically analogous to its Floquet counterpart. Some of the extraordinary results of Floquet-engineering, such as the sign reversal of the exchange interaction or electronic tunneling, which are not obtained by coupling to a dark cavity, can already be realized with a single-photon state (no coherent states are needed). The analytic results are verified and extended with numerical simulations on a two-site Hubbard model coupled to a driven cavity mode. Our results generalize the well-established Floquet-engineering of correlated electrons to the regime of quantum light. It opens up a new pathway of controlling properties of quantum materials with high tunability and low energy dissipation., Comment: 20 pages, 11 figures

We investigate the equilibrium state and the collective modes of an excitonic insulator (EI) in a Fabry-P\'erot cavity. In an EI, two bands of a semiconductor or semimetal spontaneously hybridize due to the Coulomb interaction between electrons and holes, leading to the opening of a gap. The coupling to the electromagnetic field reduces the symmetry of the system with respect to phase rotations of the excitonic order parameter from $U(1)$ to $Z_2$. While the reduction to a discrete symmetry would in general lead to a gapped phase mode and enhance the stability of the ordered phase, the coupling to the cavity leaves the mean-field ground state unaffected. Its energy remains invariant under $U(1)$ phase rotations, in spite of the lower $Z_2$ symmetry imposed by the cavity. In dipolar gauge, this can be traced back to the balancing of the linear light-matter coupling and the dipolar self-interaction at zero frequency. At nonzero frequency, however, the collective excitations do reflect the lower $Z_2$ symmetry, which shows that fluctuations beyond mean-field could play a crucial role in finding the true phase at finite temperature., Comment: 13 pages, 6 figures

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.

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 $\eta$--paired condensate at low temperatures, featuring a staggered superconducting pairing field. In this conference paper, we discuss the origin of the $\eta$--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., Comment: Conference contribution; presented in the ECSN 2019 in Odessa