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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.

Density Functional Tight-Binding (DFTB), an approximative approach derived from Density Functional Theory (DFT), has the potential to pave the way for simulations of large periodic or non-periodic systems. We have specifically tailored DFTB parameters to enhance the accuracy of electronic band gap calculations in both 3D and 2D lead-iodide perovskites, at a significantly reduced computational cost relative to state-of-the-art ab initio calculations. Our electronic DFTB parameters allow computing not only the band gap but also effective masses of perovskite materials with reasonable accuracy compared to existing experimental data and state-of-the-art DFT calculations. The electronic band structures of vacancy-ordered and, lead- and iodide- deficient perovskites are also explored. Additionally, we demonstrate the efficiency of DFTB in computing electronic band alignments in perovskite heterostructures. The DFTB-based approach is anticipated to be beneficial for studying large-scale systems such as heterostructures and nanocrystals., Comment: 44 pages, 9 figures

In a well-ordered crystalline solid, insulating behaviour can arise from two mechanisms: electrons can either scatter off a periodic potential, thus forming band gaps that can lead to a band insulator, or they localize due to strong interactions, resulting in a Mott insulator. For an even number of electrons per unit cell, either band- or Mott-insulators can theoretically occur. However, unambiguously identifying an unconventional Mott-insulator with an even number of electrons experimentally has remained a longstanding challenge due to the lack of a momentum-resolved fingerprint. This challenge has recently become pressing for the layer dimerized van der Waals compound Nb$_3$Br$_8$, which exhibits a puzzling magnetic field-free diode effect when used as a weak link in Josephson junctions, but has previously been considered to be a band-insulator. In this work, we present a unique momentum-resolved signature of a Mott-insulating phase in the spectral function of Nb$_3$Br$_8$: the top of the highest occupied band along the out-of-plane dimerization direction $k_z$ has a momentum space separation of $\Delta k_z=2\pi/d$, whereas the valence band maximum of a band insulator would be separated by less than $\Delta k_z=\pi/d$, where $d$ is the average spacing between the layers. As the strong electron correlations inherent in Mott insulators can lead to unconventional superconductivity, identifying Nb$_3$Br$_8$ as an unconventional Mott-insulator is crucial for understanding its apparent time-reversal symmetry breaking Josephson diode effect. Moreover, the momentum-resolved signature employed here could be used to detect quantum phase transition between band- and Mott-insulating phases in van der Waals heterostructures, where interlayer interactions and correlations can be easily tuned to drive such transition., Comment: 9 pages, 3 figures

Non-adiabatic molecular dynamics (NAMD) has become an essential computational technique for studying the photophysical relaxation of molecular systems after light absorption. These phenomena require approximations that go beyond the Born-Oppenheimer approximation, and the accuracy of the results heavily depends on the electronic structure theory employed. Sophisticated electronic methods, however, make these techniques computationally expensive, even for medium size systems. Consequently, simulations are often performed on simplified models to interpret experimental results. In this context, a variety of techniques have been developed to perform NAMD using approximate methods, particularly Density Functional Tight Binding (DFTB). Despite the use of these techniques on large systems where ab initio methods are computationally prohibitive, a comprehensive validation has been lacking. In this work, we present a new implementation of trajectory surface hopping (TSH) combined with DFTB, utilizing non-adiabatic coupling vectors (NACVs). We selected two different systems for validation, providing an exhaustive comparison with higher-level electronic structure methods. As a case study, we simulated a system from the class of molecular motors, which has been extensively studied experimentally but remains challenging to simulate with ab initio methods due to its inherent complexity. Our approach effectively captures the key photophysical mechanism of dihedral rotation after absorption of light. Additionally, we successfully reproduce the transition from the bright to dark states observed in the time dependent fluorescence experiments, providing valuable insights into this critical part of the photophysical behavior in molecular motors.

Engineering phases of matter in cavities requires effective light-matter coupling strengths that are on the same order of magnitude as the bare system energetics, coined the ultra-strong coupling regime. For models of itinerant electron systems, which do not have discrete energy levels, a clear definition of this regime is outstanding to date. Here we argue that a change of the electronic mass exceeding $10\%$ of its bare value may serve as such a definition. We propose a quantitative computational scheme for obtaining the electronic mass in relation to its bare vacuum value and show that coupling to surface polariton modes can induce such mass changes. Our results have important implications for cavity design principles that enable the engineering of electronic properties with quantum light., Comment: 5 pages, 3 figes + Supplement: 4 pages, 1 figure

Periodic laser driving, known as Floquet engineering, is a powerful tool to manipulate the properties of quantum materials. Using circularly polarized light, artificial magnetic fields, called Berry curvature, can be created in the photon-dressed Floquet-Bloch states that form. This mechanism, when applied to 3D Dirac and Weyl systems, is predicted to lead to photon-dressed movement of Weyl nodes which should be detectable in the transport sector. The transport response of such a topological light-matter hybrid, however, remains experimentally unknown. Here, we report on the transport properties of the type-II Weyl semimetal T$\mathrm{_d}$-MoTe$_\mathrm{2}$ illuminated by a femtosecond pulse of circularly polarized light. Using an ultrafast optoelectronic device architecture, we observed injection currents and a helicity-dependent anomalous Hall effect whose scaling with laser field strongly deviate from the perturbative laws of nonlinear optics. We show using Floquet theory that this discovery corresponds to the formation of a magnetic Floquet-Weyl semimetal state. Numerical ab initio simulations support this interpretation, indicating that the light-induced motion of the Weyl nodes contributes substantially to the measured transport signals. This work demonstrates the ability to generate large effective magnetic fields ($>$ 30T) with light, which can be used to manipulate the magnetic and topological properties of a range of quantum materials.

Starting from a low-energy continuum model for the band dispersion of the $2 \times 2$ charge-ordered phase of the kagome metals $A$V$_3$Sb$_5$ ($A=$ K, Rb, Cs), we show that nematicity can develop in this state driven either by three inequivalent $1 \times 4$ charge fluctuations preemptive of a $1 \times 4$ charge order (CO), or by an actual zero momentum $d$-wave charge Pomeranchuk instability (PI). We perform a Kohn-Luttinger analysis in the particle-hole sector, which allows us to establish a criterion for the development of an attractive nematic channel near the onset of the $1 \times 4$ CO and near the $d$-wave charge PI, respectively. We derive an effective charge-fermion model for the $d$-wave PI with a nematic susceptibility given via a random phase approximation (RPA) summation. By contrast, for the finite momentum CO, the RPA scheme breaks down and needs to be improved upon by including Aslamazov-Larkin contributions to the nematic pairing vertex. We then move to the derivation of the Ginzburg-Landau potentials for the $1 \times 4$ CO and for the $d$-wave PI, and we obtain the corresponding analytical expression for the nematic susceptibility at the nematic transition temperature T $ \sim \text{T}_\text{nem}$ in both cases. Our work establishes a relation between the nematicity observed in some of the iron-based superconductors, where the nematic phase might be driven by spin fluctuations, and the vanadium-based kagome metals, where charge fluctuations likely induce nematicity. The two microscopic mechanisms we propose for the stabilization of the nematic state in $A$V$_3$Sb$_5$ are distinguishable by diffusive scattering experiments, meaning that it is possible to gauge which of the two theories, if any, is the most likely to describe this phase. Both mechanisms might also be relevant for the recently discovered titanium-based family $A$Ti$_3$Sb$_5$., Comment: Main text + Supplemental material; 14 figures in total

We investigate Floquet engineering in a sawtooth chain -- a minimal model hosting a nearly flat band endowed with nontrivial quantum geometry -- coupled to driven surface polaritons. In this paradigmatic flat band model, light-matter coupling to a flat band is enabled by quantum geometry despite the vanishing band velocity and band curvature. We show that light polarization and finite momentum transfer in polaritonic settings provide sufficient tunability to flatten or unflatten bands, with sometimes drastic band structure modifications beyond what is attainable with laser pulses in free space. Possible implications for light-driven phenomena in prototypical flat-band moir\'e or kagome materials are discussed., Comment: 8 pages, 3 figures, including a short appendix

Recent advances in the field of condensed-matter physics have unlocked the potential to realize and control emergent material phases that do not exist in thermal equilibrium. One of the most promising concepts in this regard is Floquet engineering, the coherent dressing of matter via time-periodic perturbations. However, the broad applicability of Floquet engineering to quantum materials is still unclear. For the paradigmatic case of monolayer graphene, the theoretically predicted Floquet-induced effects, despite a seminal report of the light-induced anomalous Hall effect, have been put into question. Here, we overcome this problem by using electronic structure measurements to provide direct experimental evidence of Floquet engineering in graphene. We report light-matter-dressed Dirac bands by measuring the contribution of Floquet sidebands, Volkov sidebands, and their quantum path interference to graphene's photoemission spectral function. Our results finally demonstrate that Floquet engineering in graphene is possible, paving the way for the experimental realization of the many theoretical proposals on Floquet-engineered band structures and topological phases., Comment: 4 main figures, 3 extended figures

Van der Waals (vdW) heterostructures host many-body quantum phenomena that can be tuned in situ using electrostatic gates. These gates are often microstructured graphite flakes that naturally form plasmonic cavities, confining light in discrete standing waves of current density due to their finite size. Their resonances typically lie in the GHz - THz range, corresponding to the same $\mu$eV - meV energy scale characteristic of many quantum effects in the materials they electrically control. This raises the possibility that built-in cavity modes could be relevant for shaping the low-energy physics of vdW heterostructures. However, capturing this light-matter interaction remains elusive as devices are significantly smaller than the diffraction limit at these wavelengths, hindering far-field spectroscopic tools. Here, we report on the sub-wavelength cavity electrodynamics of graphene embedded in a vdW heterostructure plasmonic microcavity. Using on-chip THz spectroscopy, we observed spectral weight transfer and an avoided crossing between the graphite cavity and graphene plasmon modes as the graphene carrier density was tuned, revealing their ultrastrong coupling. Our findings show that intrinsic cavity modes of metallic gates can sense and manipulate the low-energy electrodynamics of vdW heterostructures. This opens a pathway for deeper understanding of emergent phases in these materials and new functionality through cavity control.

Recent experimental findings reveal non-conventional fluorescence emission in biological systems devoid of conjugated bonds or aromatic compounds, termed \textit{Non-Aromatic Fluorescence} (NAF). This phenomenon is exclusive to aggregated or solid states, remaining absent in monomeric solutions. Previous studies focused on small model systems in vacuum show that the carbonyl stretching mode along with strong interaction of short hydrogen bonds (SHBs) remain the primary vibrational mode explaining NAF in these systems. In order to simulate larger model systems taking into account the effects of the surrounding environment, in this work we propose using the density functional tight-binding (DFTB) method in combination with non-adiabatic molecular dynamics (NAMD) and the mixed quantum/molecular mechanics (QM/MM) approach. We investigate the mechanism behind NAF in the crystal structure of L-pyroglutamine-ammonium, comparing it with the related non-fluorescent amino acid L-glutamine. Our results extend our previous findings to more realistic systems, demonstrating the efficiency and robustness of the proposed DFTB method in the context of NAMD in biological systems. Furthemore, due to its inherent low computational cost, this method allows for a better sampling on the non-radiative events at the conical intersection which is crucial for a complete understanding of this phenomenon. Beyond contributing to the ongoing exploration of NAF, this work paves the way for future application of this method in more complex biological systems such as amyloid aggregates, biomaterials and non-aromatic proteins.

We investigate a long-ranged coupled and non-Hermitian two-dimensional array of nanomagnets, fabricated on a thin magnetic substrate and subjected to an in-plane magnetic field. We predict topology-driven edge and corner skin effects of magnetic eigenmodes with the localization position at boundaries precisely characterized by a topological winding tuple $({\cal W}_1,{\cal W}_2)$. By varying the direction of the in-plane field, all magnon states pile up either at different edges of the array with $({\cal W}_1=\pm 1,{\cal W}_2=0)$ or $({\cal W}_1=0,{\cal W}_2=\pm 1)$, or at different corners characterized by $({\cal W}_1=\pm 1,{\cal W}_2=\pm 1)$. Exploiting the non-Hermitian topology is potentially helpful for designing useful magnonic metasurface in the future., Comment: 7 pages, 2 figures, 1 table. Comments are welcome

Inspired by the striking discovery of metastable superconductivity in $\mathrm{K}_3\mathrm{C}_{60}$ at 100K, far above $T_{\textrm{c}}=20K$, we discuss possible mechanisms for long-lived, photo-induced superconductivity. Starting from a model of optically-driven Raman phonons coupled to inter-band electronic transitions, we develop a microscopic mechanism for photo-controlling the pairing interaction. Leveraging this mechanism, we first investigate long-lived superconductivity arising from the thermodynamic metastable trapping of the driven phonon. We then propose an alternative route, where the superconducting gap created by an optical drive leads to a dynamical bottleneck in the equilibration of quasi-particles. We conclude by discussing implications of both scenarios for experiments that can be used to discriminate between them. Our work provides falsifiable explanations for the nanosecond-scale photo-induced superconductivity found in $\mathrm{K}_3\mathrm{C}_{60}$, while simultaneously offering a theoretical basis for exploring metastable superconductivity in other quantum materials., Comment: 15 pages, 5 figures; significant update from v1

The interplay of electronic and nuclear degrees of freedom presents an outstanding problem in condensed matter physics and chemistry. Computational challenges arise especially for large systems, long time scales, in nonequilibrium, or in systems with strong correlations. In this work, we show how downfolding approaches facilitate complexity reduction on the electronic side and thereby boost the simulation of electronic properties and nuclear motion - in particular molecular dynamics (MD) simulations. Three different downfolding strategies based on constraining, unscreening, and combinations thereof are benchmarked against full density functional calculations for selected charge density wave (CDW) systems, namely 1H-TaS$_2$, 1T-TiSe$_2$, 1H-NbS$_2$, and a one-dimensional carbon chain. We find that the downfolded models can reproduce potential energy surfaces on supercells accurately and facilitate computational speedup in MD simulations by about five orders of magnitude in comparison to purely ab initio calculations. For monolayer 1H-TaS$_2$ we report classical replica exchange and quantum path integral MD simulations, revealing the impact of thermal and quantum fluctuations on the CDW transition.

Optical driving of materials has emerged as a versatile tool to control their properties, with photo-induced superconductivity being among the most fascinating examples. In this work, we show that light or lattice vibrations coupled to an electronic interband transition naturally give rise to electron-electron attraction that may be enhanced when the underlying boson is driven into a non-thermal state. We find this phenomenon to be resonantly amplified when tuning the boson's frequency close to the energy difference between the two electronic bands. This result offers a simple microscopic mechanism for photo-induced superconductivity and provides a recipe for designing new platforms in which light-induced superconductivity can be realized. We propose a concrete setup consisting of a graphene-hBN-SrTiO$_3$ heterostructure, for which we estimate a superconducting $T_{\rm c}$ that may be achieved upon driving the system.

Kagome metals $A$V$_3$Sb$_5$ ($A=$K, Rb, Cs) exhibit an exotic charge order (CO), involving three order parameters, with broken translation and time-reversal symmetries compatible with the presence of orbital currents. The properties of this phase are still intensely debated, and it is unclear if the origin of the CO is mainly due to electron-electron or electron-phonon interactions. Most of the experimental studies confirm the nematicity of this state, a feature that might be enhanced by electronic correlations. However, it is still unclear whether the nematic CO becomes stable at a temperature equal to ($T_{\text{nem}} = T_\text{C}$) or lower than ($T_{\text{nem}} < T_\text{C}$) the one of the CO itself. Here, we systematically characterize several CO configurations, some proposed for the new member of the family ScV$_6$Sn$_6$, by combining phenomenological Ginzburg-Landau theories, valid irrespective of the specific ordering mechanism, with mean-field analysis. We find a few configurations for the CO that are in agreement with most of the experimental findings to date and that are described by different Ginzburg-Landau potentials. We propose to use resonant ultrasound spectroscopy to experimentally characterize the order parameters of the CO, such as the number of their components and their relative amplitude, and provide an analysis of the corresponding elastic tensors. This might help understand which mean-field configuration found in our study is the most representative for describing the CO state of kagome metals, and it can provide information regarding the nematicity onset temperature $T_\text{nem}$ with respect to $T_\text{C}$., Comment: 16 pages, 4 figures + supplemental material (2 pages)

The hybridization between light and matter forms the basis to achieve cavity control over quantum materials. In this work we investigate a cavity coupled to an XXZ quantum chain of interacting spinless fermions by numerically exact solutions and perturbative analytical expansions. We find two important effects: (i) Specific quantum fluctuations of the matter system play a pivotal role in achieving entanglement between light and matter; and (ii) in turn, light-matter entanglement is the key ingredient to modify electronic properties by the cavity. We hypothesize that quantum fluctuations of those matter operators to which the cavity modes couple are a general prerequisite for light-matter entanglement in the groundstate. Implications of our findings for light-matter-entangled phases, cavity-modified phase transitions in correlated systems, and measurement of light-matter entanglement through Kubo response functions are discussed.

We study whether neural quantum states based on multi-layer feed-forward networks can find ground states which exhibit volume-law entanglement entropy. As a testbed, we employ the paradigmatic Sachdev-Ye-Kitaev model. We find that both shallow and deep feed-forward networks require an exponential number of parameters in order to represent the ground state of this model. This demonstrates that sufficiently complicated quantum states, although being physical solutions to relevant models and not pathological cases, can still be difficult to learn to the point of intractability at larger system sizes. This highlights the importance of further investigations into the physical properties of quantum states amenable to an efficient neural representation.

We propose a generic scenario for metastability and excitation-induced switching in layered materials. Focusing on a minimal bilayer stack, where each layer consists of a honeycomb lattice with A and B sublattices, we map out the energy landscape with respect to the relative sliding of the layers. The sliding affects the interlayer hopping, which induces a splitting between bonding and anti-bonding bands. When this splitting is large, the AA and AB stacking configurations correspond to the global and secondary minima, respectively, and these configurations are separated by a barrier against layer-sliding. While chemical doping only flattens this barrier, strong \emph{photodoping} from bonding to antibonding bands can transiently destabilize the global minimum and induce a sliding motion toward the AB stacked configuration, thereby switching from an equilibrium insulator to a nearly gapless metastable phase. This hopping-driven effect is enhanced by local repulsive interactions, which increase the gap and facilitate the inter-layer sliding., Comment: 11 pages, including paper + appendix

Many-body entanglement in condensed matter systems can be diagnosed from equilibrium response functions through the use of entanglement witnesses and operator-specific quantum bounds. Here, we investigate the applicability of this approach for detecting entangled states in quantum systems driven out of equilibrium. We use a multipartite entanglement witness, the quantum Fisher information, to study the dynamics of a paradigmatic fermion chain undergoing a time-dependent change of the Coulomb interaction. Our results show that the quantum Fisher information is able to witness distinct signatures of multipartite entanglement both near and far from equilibrium that are robust against decoherence. We discuss implications of these findings for probing entanglement in light-driven quantum materials with time-resolved optical and x-ray scattering methods., Comment: 8 pages, 4 figures

Controlling edge states of topological magnon insulators is a promising route to stable spintronics devices. However, to experimentally ascertain the topology of magnon bands is a challenging task. Here we derive a fundamental relation between the light-matter coupling and the quantum geometry of magnon states. This allows to establish the two-magnon Raman circular dichroism as an optical probe of magnon topology in honeycomb magnets, in particular of the Chern number and the topological gap. Our results pave the way for interfacing light and topological magnons in functional quantum devices., Comment: 6 pages, 3 figures, 2 tables

We study the Hatano-Nelson model, i.e., a one-dimensional non-Hermitian chain of spinless fermions with nearest-neighbour nonreciprocal hopping, in the presence of repulsive nearest-neighbour interactions. At half filling, we find two $\mathcal{PT}$ transitions, as the interaction strength increases. The first transition is marked by an exceptional point between the first and the second excited state in a finite-size system and is a first-order symmetry-breaking transition into a charge-density wave regime. Persistent currents characteristic of the Hatano-Nelson model abruptly vanish at the transition. The second transition happens at a critical interaction strength that scales with the system size and can thus only be observed in finite-size systems. It is characterized by a collapse of all energy eigenvalues onto the real axis. We further show that in a strong interaction regime, but away from half filling, the many-body spectrum shows point gaps with nontrivial winding numbers, akin to the topological properties of the single-particle spectrum of the Hatano-Nelson chain, which indicates the skin effect of extensive many-body eigenstates under open boundary conditions. Our results can be applied to other models such as the non-Hermitian Su-Schrieffer-Heeger-type model and contribute to an understanding of fermionic many-body systems with non-Hermitian Hamiltonians., Comment: 7+12 pages, 4+12 figures

Pump-probe experiments have suggested the possibility to control electronic correlations by driving infrared-active phonons with resonant midinfrared laser pulses. In this work we study two possible microscopic nonlinear electron-phonon interactions behind these observations, namely coupling of the squared lattice displacement either to the electronic density or to the double occupancy. We investigate whether photon-phonon coupling to quantized light in an optical cavity enables similar control over electronic correlations. We first show that inside a dark cavity electronic interactions increase, ruling out the possibility that $T_c$ in superconductors can be enhanced via effectively decreased electron-electron repulsion through nonlinear electron-phonon coupling in a cavity. We further find that upon driving the cavity, electronic interactions decrease. Two different regimes emerge: (i) a strong coupling regime where the phonons show a delayed response at a time proportional to the inverse coupling strength, and (ii) an ultra-strong coupling regime where the response is immediate when driving the phonon polaritons resonantly. We further identify a distinctive feature in the electronic spectral function when electrons couple to phonon polaritons involving an infrared-active phonon mode, namely the splitting of the shake-off band into three bands. This could potentially be observed by angle-resolved photoemission spectroscopy.

The emergent field of cavity quantum materials bridges collective many-body phenomena in solid-state platforms with strong light-matter coupling in cavity quantum electrodynamics (cavity QED). This brief review provides an overview of the state of the art of cavity platforms and highlights recent theoretical proposals and first experimental demonstrations of cavity control of collective phenomena in quantum materials. This encompasses light-matter coupling between electrons and cavity modes, cavity superconductivity, cavity phononics and ferroelectricity, correlated systems in a cavity, light-magnon coupling, cavity topology and the quantum Hall effect, as well as superradiance. An outlook of potential future developments is given., Comment: 14 pages, 8 figures

In a previous work [Phys. Rev. Lett. 123, 047202 (2019)] a translationally invariant framework called quantum-electrodynamical Bloch (QED-Bloch) theory was introduced for the description of periodic materials in homogeneous magnetic fields and strongly coupled to the quantized photon field in the optical limit. For such systems, we show that QED-Bloch theory predicts the existence of fractal polaritonic spectra as a function of the cavity coupling strength. In addition, for the energy spectrum as a function of the relative magnetic flux we find that a terahertz cavity can modify the standard Hofstadter butterfly. In the limit of no quantized photon field, QED-Bloch theory captures the well-known fractal spectrum of the Hofstadter butterfly and can be used for the description of 2D materials in strong magnetic fields, which are of great experimental interest. As a further application, we consider Landau levels under cavity confinement and show that the cavity alters the quantized Hall conductance and that the Hall plateaus are modified as $\sigma_{xy}=e^2\nu/h(1+\eta^2)$ by the light-matter coupling $\eta$. Most of the aforementioned phenomena should be experimentally accessible and corresponding implications are discussed.

Recent experimental advances enable the manipulation of quantum matter by exploiting the quantum nature of light. However, paradigmatic exactly solvable models, such as the Dicke, Rabi or Jaynes-Cummings models for quantum-optical systems, are scarce in the corresponding solid-state, quantum materials context. Focusing on the long-wavelength limit for the light, here, we provide such an exactly solvable model given by a tight-binding chain coupled to a single cavity mode via a quantized version of the Peierls substitution. We show that perturbative expansions in the light-matter coupling have to be taken with care and can easily lead to a false superradiant phase. Furthermore, we provide an analytical expression for the groundstate in the thermodynamic limit, in which the cavity photons are squeezed by the light-matter coupling. In addition, we derive analytical expressions for the electronic single-particle spectral function and optical conductivity. We unveil quantum Floquet engineering signatures in these dynamical response functions, such as analogs to dynamical localization and replica side bands, complementing paradigmatic classical Floquet engineering results. Strikingly, the Drude weight in the optical conductivity of the electrons is partially suppressed by the presence of a single cavity mode through an induced electron-electron interaction.

A deeper theoretical understanding of driven-dissipative interacting systems and their nonequilibrium phase transitions is essential both to advance our fundamental physics understanding and to harness technological opportunities arising from optically controlled quantum many-body states. This paper provides a numerical study of dynamical phases and the transitions between them in the nonequilibrium steady state of the prototypical two-dimensional Heisenberg antiferromagnet with drive and dissipation. We demonstrate a nonthermal transition that is characterized by a qualitative change in the magnon distribution, from subthermal at low drive to a generalized Bose-Einstein form including a nonvanishing condensate fraction at high drive. A finite-size analysis reveals static and dynamical critical scaling at the transition, with a discontinuous slope of the magnon number versus driving field strength and critical slowing down at the transition point. Implications for experiments on quantum materials and polariton condensates are discussed., Comment: 14 pages, 8 figures, with supplementary information

We propose a measurement scheme to directly detect odd-frequency superconductivity via time- and angle-resolved photoelectron fluctuation spectroscopy. The scheme includes two consecutive, non-overlapping probe pulses applied to a superconducting sample. The photoemitted electrons are collected in a momentum-resolved fashion. Correlations between signals with opposite momenta are analyzed. Remarkably, these correlations are directly proportional to the absolute square of the time-ordered anomalous Green's function of the superconductor. This setup allows for the direct detection of the "hidden order parameter" of odd-frequency pairing. We illustrate this general scheme by analyzing the signal for the prototypical case of a two-band superconductor.

Neural-network quantum states (NQS) have been shown to be a suitable variational ansatz to simulate out-of-equilibrium dynamics in two-dimensional systems using time-dependent variational Monte Carlo (t-VMC). In particular, stable and accurate time propagation over long time scales has been observed in the square-lattice Heisenberg model using the Restricted Boltzmann machine architecture. However, achieving similar performance in other systems has proven to be more challenging. In this article, we focus on the two-leg Heisenberg ladder driven out of equilibrium by a pulsed excitation as a benchmark system. We demonstrate that unmitigated noise is strongly amplified by the nonlinear equations of motion for the network parameters, which causes numerical instabilities in the time evolution. As a consequence, the achievable accuracy of the simulated dynamics is a result of the interplay between network expressiveness and measures required to remedy these instabilities. We show that stability can be greatly improved by appropriate choice of regularization. This is particularly useful as tuning of the regularization typically imposes no additional computational cost. Inspired by machine learning practice, we propose a validation-set based diagnostic tool to help determining optimal regularization hyperparameters for t-VMC based propagation schemes. For our benchmark, we show that stable and accurate time propagation can be achieved in regimes of sufficiently regularized variational dynamics., Comment: 27 pages, 13 figures

We introduce the magnon circular photogalvanic effect enabled by stimulated Raman scattering. This provides an all-optical pathway to the generation of directed magnon currents with circularly polarized light in honeycomb antiferromagnetic insulators. The effect is the leading order contribution to magnon photocurrent generation via optical fields. Control of the magnon current by the polarization and angle of incidence of the laser is demonstrated. Experimental detection by sizeable inverse spin Hall voltages in platinum contacts is proposed., Comment: 6 pager, 4 figures

Motivated by recent experimental progress we revisit the theory of pump-probe time- and angle-resolved photoemission spectroscopy (trARPES), which is one of the most powerful techniques to trace transient pump-driven modifications of the electronic properties. The pump-induced dynamics can be described in different gauges for the light-matter interaction. Standard minimal coupling leads to the velocity gauge, defined by linear coupling to the vector potential. In the context of tight-binding (TB) models, the Peierls substitution is the commonly employed scheme for single-band models. Multi-orbital extensions -- including the coupling of the dipole moments to the electric field -- have been introduced and tested recently. In this work, we derive the theory of time-resolved photoemission within both gauges from the perspective of nonequilibrium Green's functions. This approach naturally incorporates the photoelectron continuum, which allows for a direct calculation of the observable photocurrent. Following this route we introduce gauge-invariant expressions for the time-resolved photoemission signal. The theory is applied to graphene pumped with short terahertz pulses, which we treat within a first-principles TB model. We investigate the gauge invariance and discuss typical effects observed in subcycle time-resolved photoemission. Our formalism is an ideal starting point for realistic trARPES simulations including scattering effects., Comment: 12 pages, 7 figures; update reference list

Recent measurements of the resistivity in magic-angle twisted bilayer graphene near the superconducting transition temperature show two-fold anisotropy, or nematicity, when changing the direction of an in-plane magnetic field [Cao \textit{et al.}, Science \textbf{372}, 264 (2021)]. This was interpreted as strong evidence for exotic nematic superconductivity instead of the widely proposed chiral superconductivity. Counter-intuitively, we demonstrate that in two-dimensional chiral superconductors the in-plane magnetic field can hybridize the two chiral superconducting order parameters to induce a phase that shows nematicity in the transport response. Its paraconductivity is modulated as $\cos(2\theta_{\bf B})$, with $\theta_{\bf B}$ being the direction of the in-plane magnetic field, consistent with experiment in twisted bilayer graphene. We therefore suggest that the nematic response reported by Cao \textit{et al.} does not rule out a chiral superconducting ground state., Comment: 6 pages, 2 figures

The Doppler shift of the quasiparticle dispersion by charge currents is responsible for the critical supercurrents in superconductors and instabilities of the magnetic ground state of metallic ferromagnets. Here we predict an analogous effect in thin films of magnetic insulators in which microwaves emitted by a proximity stripline generate coherent chiral spin currents that cause a Doppler shift in the magnon dispersion. The spin-wave instability is suppressed by magnon-magnon interactions that limit spin currents to values close to but below the threshold for the instability. The spin current limitations by the backaction of magnon currents on the magnetic order should be considered as design parameters in magnonic devices., Comment: 6 pages, 4 figures

Under the action of coherent periodic driving a generic quantum system will undergo Floquet heating and continously absorb energy until it reaches a featureless thermal state. The phase-space constraints induced by certain symmetries can, however, prevent this and allow the system to dynamically form robust steady states with off-diagonal long-range order. In this work, we take the Hubbard model on an arbitrary lattice with arbitrary filling and, by simultaneously diagonalising the two possible SU(2) symmetries of the system, we analytically construct the correlated steady states for different symmetry classes of driving. This construction allows us to make verifiable, quantitative predictions about the long-range particle-hole and spin-exchange correlations that these states can possess. In the case when both SU(2) symmetries are preserved in the thermodynamic limit we show how the driving can be used to form a unique condensate which simultaneously hosts particle-hole and spin-wave order., Comment: 9 pages, 5 figures

Optical control of chirality in chiral superconductors bears potential for future topological quantum computing applications. When a chiral domain is written and erased by a laser spot, the Majorana modes around the domain can be manipulated on ultrafast time scales. Here we study topological superconductors with two chiral order parameters coupled via light fields by a time-dependent real-space Ginzburg-Landau approach. Continuous optical driving, or the application of supercurrent, hybridizes the two chiral order parameters, allowing one to induce and control the superconducting state beyond what is possible in equilibrium. We show that superconductivity can even be enhanced if the mutual coupling between two order parameters is sufficiently strong. Furthermore, we demonstrate that short optical pulses with spot size larger than a critical one can overcome a counteracting diffusion effect and write, erase, or move chiral domains. Surprisingly, these domains are found to be stable, which might enable optically programmable quantum computers in the future., Comment: 6 pages, 3 figures; updated version with discussion of substrate/phonon effects

Charge neutrality and their expected itinerant nature makes excitons potential transmitters of information. However, exciton mobility remains inaccessible to traditional optical experiments that only create and detect excitons with negligible momentum. Here, using angle-resolved photoemission spectroscopy, we detect dispersing excitons in the quasi-one-dimensional metallic trichalcogenide, TaSe3. The low density of conduction electrons and the low dimensionality in TaSe3 combined with a polaronic renormalization of the conduction band and the poorly screened interaction between these polarons and photo-induced valence holes leads to various excitonic bound states that we interpret as intrachain and interchain excitons, and possibly trions. The thresholds for the formation of a photo-hole together with an exciton appear as side valence bands with dispersions nearly parallel to the main valence band, but shifted to lower excitation energies. The energy separation between side and main valence bands can be controlled by surface doping, enabling the tuning of certain exciton properties., Comment: 18 pages, 4 figures, modified version. Nat. Mater. (2022)

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

Driving a two-dimensional Mott insulator with circularly polarized light breaks time-reversal and inversion symmetry, which induces an optically-tunable synthetic scalar spin chirality interaction in the effective low-energy spin Hamiltonian. Here, we show that this mechanism can stabilize topological magnon excitations in honeycomb ferromagnets and in optical lattices. We find that the irradiated quantum magnet is described by a Haldane model for magnons that hosts topologically-protected edge modes. We study the evolution of the magnon spectrum in the Floquet regime and via time propagation of the magnon Hamiltonian for a slowly varying pulse envelope. Compared to similar but conceptually distinct driving schemes based on the Aharanov-Casher effect, the dimensionless light-matter coupling parameter $\lambda = eEa/\hbar\omega$ at fixed electric field strength is enhanced by a factor $\sim 10^5$. This increase of the coupling parameter allows to induce a topological gap of the order of $\Delta \approx 2$ meV with realistic laser pulses, bringing an experimental realization of light-induced topological magnon edge states within reach., Comment: 21 pages, 4 figures

We investigate the dynamics of chiral edge states in topological polariton systems under laser driving. Using a model system comprised of topolgically trivial excitons and photons with a chiral coupling proposed by Karzig et al. [Phys. Rev. X 5, 031001 (2015)], we investigate the real-time dynamics of a lattice version of this model driven by a laser pulse. By analyzing the time- and momentum-resolved spectral function, measured by time- and angle-resolved photoluminescence in analogy with time- and angle-resolved photoemission spectroscopy in electronic systems, we find that polaritonic states in a ribbon geometry are selectively excited via their resonance with the pump laser photon frequency. This selective excitation mechanism is independent of the necessity of strong laser pumping and polariton condensation. Our work highlights the potential of time-resolved spectroscopy as a complementary tool to real-space imaging for the investigation of topological edge state engineering in devices., Comment: 8 pages, 5 figures

Pumping graphene with circularly polarized light is the archetype of light-tailoring topological bands. Realizing the induced Floquet-Chern insulator state and tracing clear experimental manifestions has been a challenge, and it has become clear that scattering effects play a crucial role. We tackle this gap between theory and experiment by employing microscopic quantum kinetic calculations including realistic electron-electron and electron-phonon scattering. Our theory provides a direct link to the build-up of the Floquet-Chern insulator state in light-driven graphene and its detection in time- and angle-resolved photoemission spectroscopy (ARPES). This allows us to study the stability of the Floquet features due to dephasing and thermalization effects. We also discuss the ultrafast Hall response in the laser-heated state. Furthermore, the induced pseudospin texture and the associated Berry curvature gives rise to momentum-dependent orbital magnetization, which is reflected in circular dichroism in ARPES (CD-ARPES). Combining our nonequilibrium calculations with an accurate one-step theory of photoemission allows us to establish a direct link between the build-up of the topological state and the dichroic pump-probe photoemission signal. The characteristic features in CD-ARPES are further corroborated to be stable against heating and dephasing effects. Thus, tracing circular dichroism in time-resolve photoemission provides new insights into transient topological properties., Comment: 16 pages, 8 figures

Chiral spin pumping is the generation of a unidirectional spin current in half of ferromagnetic films or conductors by dynamic dipolar stray fields from close-by nanomagnets. We formulate a general theory of long-range chiral interactions between magnets mediated by unidirectional traveling waves, e.g., spin waves in a magnetic film or microwaves in a waveguide. The traveling waves emitted by an excited magnet can be perfectly trapped by a second, initially passive, magnet by a dynamical interference effect. When both magnets are excited by a uniform microwave, the chiral interaction between them creates a large imbalance in their magnon numbers., Comment: PRB accepted version, 9 pages, 5 figures

Fermi surface is at the heart of our understanding of metals and strongly correlated many-body systems. An abrupt change in the Fermi surface topology, also called Lifshitz transition, can lead to the emergence of fascinating phenomena like colossal magnetoresistance and superconductivity. While Lifshitz transitions have been demonstrated for a broad range of materials by equilibrium tuning of macroscopic parameters such as strain, doping, pressure and temperature, a non-equilibrium dynamical route toward ultrafast modification of the Fermi surface topology has not been experimentally demonstrated. Combining time-resolved multidimensional photoemission spectroscopy with state-of-the-art TDDFT+$U$ simulations, we introduce a novel scheme for driving an ultrafast Lifshitz transition in the correlated type-II Weyl semimetal T$\mathrm{_{d}}$-MoTe$_{2}$. We demonstrate that this non-equilibrium topological electronic transition finds its microscopic origin in the dynamical modification of the effective electronic correlations. These results shed light on a novel ultrafast scheme for controlling the Fermi surface topology in correlated quantum materials.

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 wavepacket spreading after a single spin flip in prototypical two-dimensional ferromagnetic and antiferromagnetic quantum spin systems. We find characteristic spatial magnon density profiles: While the ferromagnet shows a square-shaped pattern reflecting the underlying lattice structure, as exhibited by quantum walkers, the antiferromagnet shows a circular-shaped pattern which hides the lattice structure and instead resembles a classical wave pattern. We trace these fundamentally different behaviors back to the distinctly different magnon energy-momentum dispersion relations and also provide a real-space interpretation. Our findings point to new opportunities for real-time, real-space imaging of quantum magnets both in materials science and in quantum simulators., Comment: 10 pages, 8 figures; title changed with respect to previous version

The role of the crystal lattice for the electronic properties of cuprates and other high-temperature superconductors remains controversial despite decades of theoretical and experimental efforts. While the paradigm of strong electronic correlations suggests a purely electronic mechanism behind the insulator-to-metal transition, recently the mutual enhancement of the electron-electron and the electron-phonon interaction and its relevance to the formation of the ordered phases have also been emphasized. Here, we combine polarization-resolved ultrafast optical spectroscopy and state-of-the-art dynamical mean-field theory to show the importance of the crystal lattice in the breakdown of the correlated insulating state in an archetypal undoped cuprate. We identify signatures of electron-phonon coupling to specific fully-symmetric optical modes during the build-up of a three-dimensional metallic state that follows charge photodoping. Calculations for coherently displaced crystal structures along the relevant phonon coordinates indicate that the insulating state is remarkably unstable toward metallization despite the seemingly large charge-transfer energy scale. This hitherto unobserved insulator-to-metal transition mediated by fully-symmetric lattice modes can find extensive application in a plethora of correlated solids.

We investigate the light-cone-like spread of electronic correlations in a laser-driven quantum chain. Using the time-dependent density matrix renormalization group, we show that high-frequency driving leads to a Floquet-engineered spread velocity that determines the enhancement of density-density correlations when the ratio of potential and kinetic energies is effectively increased both by either a continuous or a pulsed drive. For large times we numerically show the existence of a Floquet steady state at not too long distances on the lattice with minimal heating. Intriguingly, we find a discontinuity of dynamically scaled correlations at the edge of the light cone, akin to the discontinuity known to exist for quantum quenches in Luttinger liquids. Our work demonstrates the potential of pump-probe experiments for investigating light-induced correlations in low-dimensional materials and puts quantitative speed limits on the manipulation of long-ranged correlations through Floquet engineering., Comment: 9 pages, 6 figures

Using the partition-free time-dependent Landauer-B{\"u}ttiker formalism for transient current correlations, we study the traversal times taken for electrons to cross graphene nanoribbon (GNR) molecular junctions. We demonstrate electron traversal signatures that vary with disorder and orientation of the GNR. These findings can be related to operational frequencies of GNR-based devices and their consequent rational design.

We investigate the topological properties of Floquet-engineered twisted bilayer graphene above the magic angle driven by circularly polarized laser pulses. Employing a full Moir\'e-unit-cell tight-binding Hamiltonian based on first-principles electronic structure we show that the band topology in the bilayer, at twisting angles above 1.05$^\circ$, essentially corresponds to the one of single-layer graphene. However, the ability to open topologically trivial gaps in this system by a bias voltage between the layers enables the full topological phase diagram to be explored, which is not possible in single-layer graphene. Circularly polarized light induces a transition to a topologically nontrivial Floquet band structure with the Berry curvature of a Chern insulator. Importantly, the twisting allows for tuning electronic energy scales, which implies that the electronic bandwidth can be tailored to match realistic driving frequencies in the ultraviolet or mid-infrared photon-energy regimes. This implies that Moir\'e superlattices are an ideal playground for combining twistronics, Floquet engineering, and strongly interacting regimes out of thermal equilibrium., Comment: 14 pages, 9 figures, including appendix