arXiv subjects

Enrico Perfetto

Publications and source records attributed to Enrico Perfetto.

At least 19 recordsLinked to original sources

arXiv2026

Quasiparticle phono-conversion: filming carriers coalescing into excitons

Condensed matter physics is replete with phenomena involving high-energy free particles coalescing into low-energy bound few-particle states. While the cooling of the individual particles is well understood, the crucial step by which cold free carriers form a bound state remains elusive, involving complex energy and momentum relaxation pathways. Here, by combining ultrafast time- and momentum-resolved photoemission spectroscopy on a monolayer WSe$_2$ with the first-principles excitonic-Bloch equations, we resolve the conversion of initially free electrons and holes at the bandedges into bound excitons. With unprecedented energy resolution, we observe the transient \textit{coexistence} of free-carrier and excitonic bands, accompanied by a transfer of spectral weight between the two. We establish the phononic origin of exciton formation and ascribe this coexistence to a sequential relaxation cascade toward the lowest-energy excitonic states, wherein intermediate states remain weakly populated. The efficiency of this process is controlled by valley multiplicity, large-momentum phonon emission and spin-flip processes. By elucidating how bound states emerge from their elementary constituents, our results point to strategies for engineering exciton formation, with direct implications for optical materials and devices that operate with excitons or free carriers.

cond-mat.mtrl-sci↗

arXiv2026

Excitonic effects in the photocarriers dynamics of two-dimensional materials

We investigate the role of excitonic correlations in shaping the ultrafast dynamics of photoexcited carriers in semiconductors. Conventional approaches describe relaxation within single-particle frameworks, where electron-electron and electron-phonon scattering drive thermalization toward Fermi-Dirac distributions, neglecting electron-hole correlations that dominate near band edges. We introduce a two-particle framework based on excitonic Bloch equations (XBE) that captures carrier-phonon scattering and explicitly accounts for exciton formation. Applying this approach to non-resonantly photoexcited WSe$_2$ monolayers, we reveal qualitatively different carrier relaxation pathways: in contrast to state-of-the-art methods, XBE predict enhanced intervalley scattering and dominant carrier population in Q valleys over K valleys, in agreement with time-resolved ARPES experiments. Moreover, the momentum distribution of thermalized carriers is shaped by exciton wavefunctions rather than by Fermi-Dirac statistics, signaling the formation of a correlated nonequilibrium state. These results establish excitonic correlations as a key mechanism governing photocarrier dynamics in excitonic materials.

cond-mat.mtrl-sci↗

arXiv2026

Excitonic Mott transition without population inversion

Exciton dissociation via the excitonic Mott transition (EMT) governs the high-density optical response of semiconductors and sets fundamental limits for optoelectronic devices. The EMT is conventionally linked to the onset of population inversion and the emergence of optical gain. Here, we demonstrate that this paradigm can break down under ultrafast non-equilibrium excitation. Using femtosecond pump-probe optical spectroscopy, we drive a monolayer transition metal dichalcogenide into a dense photoexcited state in which the excitonic resonance is completely quenched within ~100 fs, while the optical gain is entirely absent across the explored fluence range. State-of-the-art real-time ab initio simulations reveal that the EMT is governed by an interplay of strongly nonthermal carrier populations and nonequilibrium dynamical screening of the Coulomb interaction. The quantitative agreement between theory and experiment identifies a distinct, ultrafast pathway to exciton ionization beyond quasi-equilibrium descriptions and demonstrates that population inversion is not a universal prerequisite for the EMT.

cond-mat.mes-hall↗

arXiv2026

Ultrafast nonlinear Hall effect in black phosphorus

The nonlinear Hall effect (NHE) is a recently discovered member of the Hall effect family in which the Hall voltage shows a nonlinear behavior when a transverse electric field is applied. While the NHE does not require broken time-reversal symmetry, such as that induced by a magnetic field, it requires broken inversion symmetry, which limits the range of suitable systems and potential applications. Here, we demonstrate an ultrafast NHE in centrosymmetric black phosphorus through dynamical symmetry breaking using femtosecond light pulses. We provide a detailed microscopic picture of excited carrier dynamics and induced fields using momentum-resolved photoemission spectroscopy combined with \textit{ab-initio} calculations. The ultrafast NHE is observed exclusively for the light polarization aligned with the armchair high-symmetry direction and persists over 300 fs, which opens new possibilities for selective and ultrafast light-to-current conversions.

cond-mat.mtrl-sci↗

arXiv2026

Many-Body Perturbation Theory for Driven Dissipative Quasiparticle Flows and Fluctuations

We present a unified many-body perturbation theory for open quantum systems, that treats dissipation, correlations, and external driving on equal footing. Using a Keldysh-Lindblad formalism, we introduce diagrammatic treatment of dissipative interaction lines representing quasiparticle flows and fluctuations. Two new Feynman rules render the evaluation of dissipative diagrams compact and systematically improvable, while preserving the Keldysh and anti-Hermitian symmetries of the closed-system theory. Consequently, the structure of the Kadanoff-Baym equations (KBE) remains unchanged, enabling existing numerical methods to be directly applied. To illustrate this, we derive dissipative versions of the second Born and $GW$ approximations, identifying the physical content of the self-energy components. Moreover, we demonstrate that time-linear approximations to the full KBE retain their closed structure and can be efficiently used to simulate relaxation and decoherence dynamics. The impact of dissipation-induced correlations is illustrated in the driven Haldane model, where quasiparticles exhibit nontrivial stabilization and acquire lifetimes that far exceed those of the bare system. This framework establishes a general route toward first-principles modeling of correlated, driven, and dissipative quantum materials.

cond-mat.str-el↗

arXiv2026

Unified First-Principles Formula for Time-Resolved ARPES Spectra of Coherent and Incoherent Excitons

Despite major experimental progresses in time-resolved and angle-resolved photoemission spectroscopy, a quantitative, microscopic framework for interpreting exciton-induced modifications of electronic band structures -- applicable even beyond the low-density limit -- is still lacking. Here we close this gap by introducing a unified approach that links the dynamics of coherent and incoherent excitons to distinct and experimentally observable excitonic sidebands. Our central result is a general, first-principles formula for time-resolved photoemission spectra, applicable across a broad range of temperatures, excitation densities, and pump-probe delays. This advance provides a predictive tool for quantitatively tracking excitonic dynamics in complex materials.

cond-mat.mtrl-sci↗

arXiv2025

Exceptional Excitons

Non-Hermitian physics is reshaping our understanding of quantum systems by revealing states and phenomena without Hermitian counterparts. While non-Hermiticity is typically associated with gain-loss processes in open systems, we uncover a fundamentally different route to non-Hermitian behavior emerging from non-equilibrium correlations. In photoexcited semiconductors, the effective interaction between electrons and holes gives rise to a pseudo-Hermitian Bethe-Salpeter Hamiltonian (PH-BSH) that governs excitonic states in the presence of excited populations. Within this framework, we identify a previously unknown class of excitonic quasiparticles - exceptional excitons - corresponding to exceptional points embedded inside the electron-hole continuum. Exceptional excitons emerge at the onset of population inversion, and represent the strongly renormalized counterparts of the system's equilibrium excitons. They are spatially localized, protected against hybridization with the continuum, and remain long-lived even in regimes where conventional excitons undergo a Mott transition. Crucially, exceptional excitons appear only when the PH-BSH is evaluated with non-thermal, resonantly generated carrier populations that support an excitonic superfluid. Ab initio results for monolayer WS_2 explicitly demonstrate this scenario and show that exceptional excitons can be realized with existing ultrafast pumping techniques. We also identify distinctive optical and photoemission signatures that enable their unambiguous detection.

cond-mat.mtrl-sci↗

arXiv2025

Non-Hermitian Bethe-Salpeter Equation for Open Systems: Emergence of Exceptional Points in Excitonic Spectra from First Principles

In open quantum systems hosting excitons, dissipation mechanisms critically shape the excitonic dynamics, band-structure and topological properties. A microscopic understanding of excitons in such non-Hermitian settings demands a first-principles generalization of the Bethe-Salpeter equation (BSE). Building on a recently introduced nonequilibrium Green's function formalism compatible with Lindbladian dynamics, we derive a non-Hermitian BSE from diagrammatic perturbation theory on the Keldysh contour, and obtain a microscopic excitonic Hamiltonian that incorporates dissipation while preserving causality. We apply the formalism to valley excitons in transition metal dichalcogenides coupled to structured photon baths. We uncover a rich landscape of exceptional points in momentum space, forming either discrete sets or continuous manifolds, depending on bath structure. The exceptional points give rise to nonanalytic valley-polarization, unusual polarization pattern in photoluminescence, and nontrivial topological signatures. Our results establish a first-principles framework for predicting and controlling excitonic behavior in open quantum materials, showing how engineered environments can be leveraged to induce and manipulate non-Hermitian and topological properties.

cond-mat.mes-hall↗

arXiv2025

A Unified Simulation Framework for Correlated Driven-Dissipative Quantum Dynamics

Time-resolved photoemission spectroscopy provides a unique and direct way to explore the real-time nonequilibrium dynamics of electrons and holes. The formal theory of the spectral function evolution requires inclusion of electronic correlations and dissipation, which are challenging due to the associated long simulation timescales which translate to a high computational cost. Recent methodological developments, namely the Real-Time Dyson Expansion, as well as theoretical developments of many-body perturbation theory for dissipative systems, have allowed for the study of driven-dissipative interacting quantum systems. In this work, we implement the hitherto unrealized study of driven-dissipative interacting quantum systems which includes driven dynamical correlations and utilizes these new methods and perturbative expansions. We illustrate the combined formalism on a prototypical two-band semiconductor model with long-range density-density Coulomb interactions. We show that the intraband thermalization of conduction band electrons induces nontrivial time-dependent changes in the system's bandstructure and a time-evolving band-gap renormalization (with a reduction by up to 10\%). We show that the qualitative features are preserved for a variety of parameters, discuss the corresponding spectral dynamics, and provide an outlook on the newly introduced simulation framework, which enables treating electron-electron scattering and dissipation effects on equal footing.

cond-mat.mtrl-sci↗

arXiv2025

The First Principles Equation for Coherent Phonons: Dynamics and Polaron distortions

This paper addresses the first principles description of coherent phonons in systems subjected to optical excitations and/or doping. We reformulate the first-principles Ehrenfest equation (fpEE) [Phys. Rev. X {\bf 13}, 031026 (2023)] in terms of Born-Oppenheimer phonon frequencies and dynamical Born effective charges. We demonstrate that nonadiabatic effects renormalize the Born-Oppenheimer frequencies and introduce a damping term responsible for the finite lifetime of coherent phonons. Notably, both the frequency renormalization and the lifetime are identical to those of quantum phonons. Furthermore, we show that electrons exert a force driven by an unconventional dynamically screened electron-phonon coupling. This coupling is smaller than the bare one even in the adiabatic limit, highlighting the need to revise current models. The fpEE is also used to develop a first-principles polaron theory that describes lattice distortions induced by doping.

cond-mat.mtrl-sci↗

arXiv2025

Long-Lived Coherence between Incoherent Excitons revealed by Time-Resolved ARPES: An Exact Solution

We investigate the exciton dynamics in an exactly solvable two-band model for semiconductors. The model incorporates light-matter, electron-electron and electron-phonon interactions, and captures exciton formation as well as the transition from the coherent to the incoherent regime. We analyze excitonic polarization, populations and coherences, with special focus on their impact in Time-Resolved and Angle-Resolved Photoemission Spectroscopy (TR-ARPES). For nonresonant pumping with below-gap photon energies, TR-ARPES spectra reveal distinct excitonic replica and quantum beats persisting in the incoherent regime. These are due to a coherence between different species of {\em incoherent} excitons. Such type of coherence is resistant to phonon dephasing, indicating that it follows different dynamics than those governing the coherences considered so far.

cond-mat.mtrl-sci↗

arXiv2025

Exact formula with two dynamically screened electron-phonon couplings for positive phonon-linewidths approximations

In this paper, we present an exact formula for the phonon linewidths involving only dressed electron-phonon couplings and ensuring the positivity property. The formula is designed to account for both nonadiabatic and correlation effects, and it provides an alternative proof that Density Functional Perturbation Theory calculations of phonon linewidths are not affected by a double counting of screening diagrams. Furthermore, we extend the treatment to nonequilibrium scenarios and offer a rigorous justification for employing the phononic Boltzmann equation.

cond-mat.mtrl-sci↗

arXiv2025

The 2025 Roadmap to Ultrafast Dynamics: Frontiers of Theoretical and Computational Modelling

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.

cond-mat.mtrl-sci↗

arXiv2024

Excitonic Bloch equations from first principles

The ultrafast conversion of coherent excitons into incoherent excitons, as well as the subsequent exciton diffusion and thermalization, are central topics in current scientific research due to their relevance in optoelectronics, photovoltaics and photocatalysis. Current approaches to the exciton dynamics rely on {\em model} Hamiltonians that depend on already screened electron-electron and electron-phonon couplings. In this work, we subject the state-of-the-art methods to scrutiny using the {\em ab initio} Hamiltonian for electrons and phonons. We offer a rigorous and intuitive proof demonstrating that the exciton dynamics governed by model Hamiltonians is affected by an overscreening of the electron-phonon interaction. The introduction of an auxiliary exciton species, termed the irreducible exciton, enables us to formulate a theory free from overscreening and derive the excitonic Bloch equations. These equations describe the time-evolution of coherent, irreducible, and incoherent excitons during and after the optical excitation. They are applicable beyond the linear regime, and predict that the total number of excitons is preserved when the external fields are switched off.

cond-mat.mtrl-sci↗

arXiv2024

Theory of coherent phonons coupled to excitons

The interaction of excitons with lattice vibrations underlies the scattering from bright to dark excitons as well as the coherent modulation of the exciton energy. Unlike the former mechanism, which involves phonons with finite momentum, the latter can be exclusively attributed to {\it coherent phonons} with zero momentum. We here lay down the microscopic theory of coherent phonons interacting with resonantly pumped bright excitons and provide the explicit expression of the corresponding coupling. The coupling notably resembles the exciton-phonon one, but with a crucial distinction: it contains the bare electron-phonon matrix elements rather than the screened ones. Our theory predicts that the exciton energy features a polaronic-like red-shift and monochromatic oscillations or beatings, depending on the number of coupled optical modes. Both the red-shift and the amplitude of the oscillations are proportional to the excitation density and to the square of the exciton-coherent-phonon coupling. We validate our analytical findings through comparisons with numerical simulations of time-resolved optical absorbance in resonantly pumped MoS$_{2}$ monolayers.

cond-mat.mes-hall↗

arXiv2023

Semiconductor Electron-Phonon Equations: a Rung Above Boltzmann in the Many-Body Ladder

Starting from the {\em ab initio} many-body theory of electrons and phonons, we go through a series of well defined simplifications to derive a set of coupled equations of motion for the electronic occupations and polarizations, nuclear displacements as well as phononic occupations and coherences. These are the semiconductor electron-phonon equations (SEPE), sharing the same scaling with system size and propagation time as the Boltzmann equations. At the core of the SEPE is the {\em mirrored} Generalized Kadanoff-Baym ansatz (GKBA) for the Green's functions, an alternative to the standard GKBA which we show to lead to unstable equilibrium states. The SEPE treat coherent and incoherent degrees of freedom on equal footing, widen the scope of the semiconductor Bloch equations and Boltzmann equations, and reduce to them under additional simplifications. The new features of the SEPE pave the way for first-principles studies of phonon squeezed states and coherence effects in time-resolved absorption and diffraction experiments.

cond-mat.mtrl-sci↗

arXiv2023

Real-time GW-Ehrenfest-Fan-Migdal method for nonequilibrium 2D materials

Quantum simulations of photoexcited low-dimensional systems are pivotal for understanding how to functionalize and integrate novel two-dimensional (2D) materials in next-generation optoelectronic devices. First principles predictions are extremely challenging due to the simultaneous interplay of light-matter, electron-electron and electron-nuclear interactions. We here present an advanced ab initio many-body method which accounts for quantum coherence and non-Markovian effects while treating electrons and nuclei on equal footing, thereby preserving fundamental conservation laws like the total energy. The impact of this advancement is demonstrated through real-time simulations of the complex multivalley dynamics in a molybdenum disulfide (MoS$_{2}$) monolayer pumped above gap. Within a single framework we provide a parameter-free description of the coherent-to-incoherent crossover, elucidating the role of microscopic and collective excitations in the dephasing and thermalization processes.

cond-mat.mes-hall↗

arXiv2023

In- and out-of-equilibrium {\em ab initio} theory of electrons and phonons

We lay down the {\em ab initio} many-body quantum theory of electrons and phonons in- and out-of-equilibrium at any temperature. We begin by addressing a fundamental issue concerning the {\em ab initio} Hamiltonian in the harmonic approximation, which we show must be determined {\em self-consistently} to avoid inconsistencies. After identifying the most suitable partitioning into a ``noninteracting'' and an ``interacting'' part we embark on the Green's function diagrammatic analysis. We single out key diagrammatic structures to carry on the expansion in terms of dressed propagators and screened interaction. The final outcome is the finite-temperature nonequilibrium extension of the Hedin equations, featuring the appearance of the time-local Ehrenfest diagram in the electronic self-energy. The Hedin equations have limited practical utility for real-time simulations of driven systems. We leverage the versatility of diagrammatic expansion to generate a closed system of integro-differential equations for the Green's functions and nuclear displacements. These are the Kadanoff-Baym equations for electrons and phonons. Another advantage of the diagrammatic derivation is the ability to use conserving approximations, which ensure the satisfaction of all fundamental conservation laws during the time evolution. As an example we show that the adiabatic Born-Oppenheimer approximation is not conserving whereas its dynamical extension is conserving provided that the electrons are treated in the Fan-Migdal approximation with a dynamically screened electron-phonon coupling. We also derive the formal solution of the Kadanoff-Baym equations in the long time limit and at the steady state. The expansion of the phononic Green's function around the quasi-phonon energies points to a possible correlation-induced splitting of the phonon dispersion in materials with no time-reversal invariance.

cond-mat.mtrl-sci↗