arXiv subjects

Daria Popova-Gorelova

Publications and source records attributed to Daria Popova-Gorelova.

16 recordsLinked to original sources

arXiv2026

Real-time exciton dynamics in two-dimensional materials under ultrashort laser pulses

The optical response of two-dimensional materials is often significantly impacted by excitonic effects due to the reduced screening of attractive Coulomb interactions in low-dimensional systems. Accurate modeling of exciton formation and real-time dynamics is essential to understanding their ultrafast optical properties. In this study, we theoretically investigate the exciton dynamics in a two-dimensional hexagonal boron nitride (h-BN) and a germanium sulfide (GeS) monolayers exposed to an ultrashort laser pulse. We analyze the system's response to the external field in one- and two-photon excitation regimes. For our calculations, we combine a state-of-the-art ab initio approach to study exciton dynamics with a highly precise numerical scheme. We incorporate electron-hole interactions through a non-local self-energy operator derived from the many-body perturbation theory (MBPT) within the time-dependent adiabatic $GW$ (TD-a$GW$) approximation. We implement this approach using the full-electron LAPW+lo method in the all-electron exciting package. Our results elucidate the role of many-body effects in shaping ultrafast excitonic processes in two-dimensional materials, contributing to the fundamental understanding necessary for optoelectronic and photonic applications.

cond-mat.mtrl-sci↗

arXiv2026

An exciting approach to theoretical spectroscopy

Theoretical spectroscopy, and more generally, electronic-structure theory, are powerful concepts for describing the complex many-body interactions in materials. They comprise a variety of methods that can capture all aspects, from ground-state properties to lattice excitations to different types of light-matter interaction, including time-resolved variants. Modern electronic-structure codes implement either a few or several of these methods. Among them, exciting is an all-electron full-potential package that has a very rich portfolio of all levels of theory, with a particular focus on excitations. It implements the linearized augmented planewave plus local orbital (LAPW+LO) basis, which is known as the gold standard for solving the Kohn-Sham equations of density-functional theory (DFT). Based on this, it also offers benchmark-quality results for a wide range of excited-state methods. In this review, we provide a comprehensive overview of the features implemented in exciting in recent years, accompanied by short summaries on the state of the art of the underlying methodologies. They comprise DFT and time-dependent DFT (TDDFT), density-functional perturbation theory (DFPT) for phonons and electron-phonon coupling, and many-body perturbation theory in terms of the $GW$ approach and the Bethe-Salpeter equation (BSE). Moreover, exciting can handle resonant inelastic x-ray scattering (RIXS), pump-probe spectroscopy as well as exciton-phonon coupling (EXPC). Finally, we cover workflows and a view on data and machine learning (ML). All aspects are demonstrated with examples for scientifically relevant materials.

cond-mat.mtrl-sci↗

arXiv2026

Femtosecond concerted rotation of molecules on a 2D material interface

Interfaces between molecules and 2D materials exhibit energy-driven functionalities, wherein charge transfer directs molecular motion. Unlike equilibrium systems, where molecular assemblies settle into static configurations, continuous energy input can drive transient, collective molecular rearrangements. Here, we reveal ultrafast spectroscopic fingerprints of a collective rotational response of molecules on a 2D material following photoexcitation. Our results suggest that photoinduced charge transfer reshapes the interfacial energy potential, giving rise to macroscopic, unidirectional molecular rotation and the formation of a homochiral molecular arrangement. Using a multiplexed ultrafast photoemission spectroscopy approach, we simultaneously track, electronic states, atomic positions, and orbital wavefunctions with femtosecond and sub-ångström resolution. Multimodal valence and core electron emission analysis disentangles the intertwined electronic-structural dynamics of the molecule and the 2D material, revealing the dynamic modulation of charge distribution and intermolecular forces that drive collective molecular motion. Our findings open a pathway for designing energy-driven molecular systems with tunable interfacial dynamics, with potential applications in chiral engineering and active matter systems.

cond-mat.mtrl-sci↗

arXiv2025

Attosecond momentum-resolved resonant inelastic x-ray scattering for imaging coupled electron-hole dynamics

Improving our understanding of electron dynamics is essential for advancing energy transfer, optoelectronics, light harvesting systems and quantum computing. Recent developments in attosecond x-ray sources provide the fundamental possibility of observing these dynamics with atomic-scale resolution. However, connecting a time-resolved signal to dynamics is challenging due to the broad bandwidth of an attosecond probe pulse. This makes exploring the capabilities of different attosecond imaging techniques crucial. Here, we propose attosecond momentum-resolved resonant inelastic x-ray scattering as a prominent technique for tracking ultrafast dynamics. We demonstrate that the scattering signal contains an information about the instantaneous distribution of charge density across the scattering atoms. To illustrate this, we consider scattering from an $α$-sexithiophene molecule, in which coupled electron-hole dynamics are excited.

physics.comp-ph↗

arXiv2025

Laser-dressed partial density of states

The manipulation of material properties by laser light holds great promise for the development of future technologies. However, the full picture of the electronic response to laser driving remains to be uncovered. We present a novel approach to reveal details of the electron dynamics of laser-dressed materials, which consists of calculating and analysing the time-dependent partial density of states (PDOS) of materials during their interaction with a driving electromagnetic field. We show that the laser-dressed PDOS provides information about the structure of the bonds that form the laser-dressed electron density, analogous to the information that a PDOS can provide about the electron structure in a field-free case. We illustrate how our method can provide insights into the electron dynamics of materials in a site- and orbital-selective manner with calculations for a laser-dressed wurtzite ZnO crystal. Our work provides an analytical tool for the interpretation of subcycle-resolved experiments on laser-dressed materials and for the development of strategies for optical manipulation of material properties.

cond-mat.mtrl-sci↗

arXiv2025

Second-order microscopic nonlinear susceptibility in a centrosymmetric material: application to imaging valence electron motion

We report measurements of phase-matched nonlinear x-ray and optical sum-frequency generation from single-crystal silicon using sub-resonant 0.95 eV laser pulses and 9.5 keV hard x-ray pulses from the LCLS free-electron laser. The sum-frequency signal appears as energy and momentum sidebands to the elastic Bragg peak. It is proportional to the magnitude squared of the relevant temporal and spatial Fourier components of the optically induced microscopic charges/currents. We measure the first- and second-order sideband to the 220 Bragg peak and find that the efficiency is maximized when the applied field is along the reciprocal lattice vector. For an optical intensity of $\sim10^{12} \text{W}/\text{cm}^2$, we measure peak efficiencies of $3\times 10^{-7}$ and $3\times 10^{-10}$ for the first and second-order sideband respectively (relative to the elastic Bragg peak). The first-order sideband is consistent with induced microscopic currents along the applied electric field (consistent with an isotropic response). The second-order sideband depends nontrivially on the optical field orientation and is consistent with an anisotropic response originating from induced charges along the bonds with C$_{3v}$ site symmetry. The results agree well with first-principles Bloch-Floquet calculations.

cond-mat.mtrl-sci↗

arXiv2024

Revealing fingerprints of valence excitons in x-ray absorption spectra with the Bethe-Salpeter equation

The Bethe-Salpeter equation (BSE) is a powerful theoretical approach that is capable to accurately treat electron-hole interactions in materials in an excited state. We developed an ab initio framework based on the BSE to describe a pump-probe experiment, in which an x-ray pulse probes solid-state valence excitons by means of x-ray absorption spectroscopy. Our theoretical framework is of relevance for an accurate modeling of pump-probe experiments of photo-excited materials that utilize novel capabilities offered by x-ray science.

cond-mat.mtrl-sci↗

arXiv2023

Attosecond imaging of photo-induced dynamics in molecules using time-resolved photoelectron momentum microscopy

We explore the novel capabilities offered by attosecond extreme ultraviolet and x-ray pulses that can be now generated by free-electron lasers and high-harmonics generation sources for probing photon-induced electron dynamics in molecules. We theoretically analyze how spatial and temporal dependence of charge migration in a pentacene molecule can be followed by means of time-resolved photoelectron microscopy on the attosecond time scale. Performing the analysis, we accurately take into account that an attosecond probe pulse leads to considerable spectral broadening. We demonstrate that the excited-state dynamics of a neutral pentacene molecule in the real space map onto unique features of photoelectron momentum maps.

quant-ph↗

arXiv2021

Heisenberg representation of nonthermal ultrafast laser excitation of magnetic precessions

We derive the Heisenberg representation of the ultrafast inverse Faraday effect that provides the time evolution of magnetic vectors of a magnetic system during its interaction with a laser pulse. We obtain a time-dependent effective magnetic operator acting in the Hilbert space of the total angular momentum that describes a process of nonthermal excitation of magnetic precessions in an electronic system by a circularly polarized laser pulse. The magnetic operator separates the effect of the laser pulse on the magnetic system from other magnetic interactions. The effective magnetic operator provides the equations of motion of magnetic vectors during the excitation by the laser. We show that magnetization dynamics calculated with these equations is equivalent to magnetization dynamics calculated with the time-dependent Schrödinger equation, which takes into account the interaction of an electronic system with the electric field of light. We model and compare laser-induced precessions of magnetic sublattices of an easy-plane and an easy-axis antiferromagnetic systems. Using these models, we show how the ultrafast inverse Faraday effect induces a net magnetic moment in antiferromagnets and demonstrate that a crystal field environment and the exchange interaction play essential roles for laser-induced magnetization dynamics even during the action of a pump pulse. Using our approach, we show that light-induced precessions can start even during the action of the pump pulse with a duration several tens times shorter than the period of induced precessions and affect the position of magnetic vectors after the action of the pump pulse.

quant-ph↗

arXiv2020

Atomic-scale imaging of laser-driven electron dynamics in solids using subcycle-resolved x-ray-optical wave mixing

We investigate laser-driven electron dynamics in solids on the atomic scale and in real space within Floquet formalism, and develop a method based on subcycle-resolved x-ray-optical wave mixing to reconstruct those dynamics. We analyze how time-reversal and inversion symmetries influence properties of optically-induced charge distributions and microscopic electron currents. Several examples for the $μ$th-order microscopic optical response of band-gap crystals are shown and compared for cases when there is either a considerable or a vanishing $μ$th-order macroscopic response. We then analyze the consequence of crystal symmetries on subcycle-resolved x-ray-optical wave mixing, a process in which an x-ray pulse of a duration shorter than the optical cycle of the driving pulse interacts with a laser-dressed crystal. Based on this analysis, we develop a method to reconstruct amplitudes and phases of Fourier components of optically-induced charge distributions from momentum and delay dependence of x-ray-optical wave-mixing spectra. Subcycle-resolved x-ray-optical wave mixing also reveals phases of temporal oscillations of microscopic optical response and some properties of microscopic laser-driven electron currents.

physics.optics↗

arXiv2020

Microscopic electron dynamics in nonlinear optical response of solids

We investigate the microscopic properties of the nonlinear optical response of crystalline solids within Floquet theory, and demonstrate that optically-induced microscopic charge distributions display complex spatial structure and nontrivial properties. Their spatial symmetry and temporal behavior are governed by crystal symmetries. We find that even when a macroscopic optical response of a crystal is forbidden, the microscopic optical response can, in fact, be nonzero. In such a case, the optically-induced charge redistribution can be considerable, even though the corresponding Fourier component of the time-dependent dipole moment per unit cell vanishes. We develop a method that makes it possible to completely reconstruct the microscopic optically-induced charge distributions by means of subcycle-resolved x-ray-optical wave mixing. We also show how, within this framework, the direction of the instantaneous microscopic optically-induced electron current flow can be revealed.

quant-ph↗

arXiv2018

Theory of x-ray scattering from laser-driven electronic systems

We describe, within the framework of quantum electrodynamics, an interaction between a non-resonant hard x-ray pulse and an electronic system in the presence of a temporally periodic laser field driving electron dynamics in this system. We apply Floquet theory to describe the laser-driven electronic system, and then obtain the scattering probability of an arbitrary nonresonant x-ray pulse from such a system employing the density-matrix formalism. We show that the scattering probability can be connected to the time-dependent electron density of the driven electronic system only under certain conditions, in particular, if the bandwidth of the probe x-ray pulse is sufficiently narrow to spectroscopically resolve transitions to different final states. A special focus is laid on application of the theory to laser-driven crystals in a strongly nonperturbative regime. We show how the time-dependent electron density of a crystal can be reconstructed from energy-resolved scattering patterns. This is illustrated by a calculation of a diffraction signal from a driven MgO crystal.

physics.optics↗

arXiv2018

Imaging Electron Dynamics with Ultrashort Light Pulses: A Theory Perspective

A wide range of ultrafast phenomena in various atomic, molecular and condense matter systems is governed by electron dynamics. Therefore, the ability to image electronic motion in real space and real time would provide a deeper understanding of such processes and guide developments of tools to control them. Ultrashort light pulses, which can provide unprecedented time resolution approaching subfemtosecond time scale, are perspective to achieve real-time imaging of electron dynamics. This task is challenging not only from an experimental view, but also from a theory perspective, since standard theories describing light-matter interaction in a stationary regime can provide erroneous results in an ultrafast case as demonstrated by several theoretical studies. We review the theoretical framework based on quantum electrodynamics, which has been shown to be necessary for an accurate description of time-resolved imaging of electron dynamics with ultrashort light pulses. We compare the results of theoretical studies of time-resolved nonresonant and resonant X-ray scattering, and time- and angle-resolved photoelectron spectroscopy and show that the corresponding time-resolved signals encode analogous information about electron dynamics. Thereby, the information about an electronic system provided by these time-resolved techniques is different from the information provided by their time-independent analogues.

physics.atom-ph↗

arXiv2016

Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet (XUV) probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into account the indistinguishability of transitions induced by the ultrashort, broadband probe pulse and electron hole correlation effects, is necessary for the interpretation of time- and angle-resolved photoelectron spectra. We show how a Fourier analysis of time- and angle-resolved photoelectron spectra from a molecule can be applied to follow its electron dynamics by considering photoelectron distributions from an indole molecular cation with coherent electron dynamics.

physics.optics↗

arXiv2015

Imaging interatomic electron current in crystals with ultrafast resonant x-ray scattering

We demonstrate how the technique of ultrafast resonant x-ray scattering can be applied to imaging dynamics of electronic wave packets in crystals. We study scattering patterns from crystals with electron dynamics in valence bands taking into account that inelastic and elastic scattering events induced by a broad-band probe pulse cannot be separated through the spectroscopy of the scattered photon. As a result, scattering patterns are not determined by the structure factor at the time of measurement, but can encode the instantaneous electron current between scattering atoms. We provide examples of how the interatomic electron current in a periodic structure can be extracted from a single scattering pattern by considering valence electron hole motion in (KBr)$_{108}$ and Ge$_{83}$ clusters.

physics.optics↗

arXiv2015

Imaging instantaneous electron flow with ultrafast resonant x-ray scattering

We propose a novel way to image dynamical properties of nonstationary electron systems using ultrafast resonant x-ray scattering. Employing a rigorous theoretical analysis within the framework of quantum electrodynamics, we demonstrate that a single scattering pattern from a nonstationary electron system encodes the instantaneous interatomic electron current in addition to the structural information usually obtained by resonant x-ray scattering from stationary systems. Thus, inelastic contributions that are indistinguishable from elastic processes induced by a broadband probe pulse, instead of being a concern, serve as an advantage for time-resolved resonant x-ray scattering. Thereby, we propose an approach combining elastic and inelastic resonant x-ray scattering for imaging dynamics of nonstationary electron systems in both real space and real time. In order to illustrate its power, we show how it can be applied to image the electron hole current in an ionized diatomic molecule.

physics.atom-ph↗