arXiv subjects

Sivan Refaely-Abramson

Publications and source records attributed to Sivan Refaely-Abramson.

At least 19 recordsLinked to original sources

arXiv2026

Application of the exact-factorization density-functional perturbation approach to pentacene crystal and monolayer MoS2

Non-adiabatic effects arising from electron-phonon interactions are often neglected within the Born-Oppenheimer (BO) approximation, which assumes that electronic states adjust instantaneously to nuclear motion. The exact factorization (EF) formalism provides a rigorous framework for treating such effects beyond the adiabatic regime and has recently been adapted to density functional theory (DFT) in the harmonic limit. Building on these foundations, we previously introduced an EF-based perturbative scheme, the EF density-functional perturbation theory (EF-DFPT), that enables the computation of phonon-driven non-adiabatic (NA) corrections to Kohn-Sham (KS) electronic states, up to second order in nuclear displacements. Here, we present the first implementation and application of EF-DFPT to extended periodic materials, focusing on its impact on experimentally relevant observables. Using the pentacene molecular crystal and monolayer MoS2 as representative soft- and stiff-mode systems, respectively, we demonstrate how NA electron-phonon interactions modify the static dielectric response. We show that these modifications originate from the combined effect of NA phonon-dressed electronic wavefunctions and second-order NA energy renormalizations. The resulting behavior is strongly material dependent: NA effects are negligible in monolayer MoS2, whereas in pentacene they lead to pronounced long-range screening effects associated with soft vibrational modes and enhanced electron-phonon coupling.

cond-mat.mtrl-sci↗

arXiv2026

Zero-phonon line emission of single photon emitters in helium-ion treated MoS$_2$

We explore the zero-phonon line of single photon emitters in helium-ion treated monolayer MoS$_2$, which are currently understood in terms of single sulfur-site vacancies. By comparing the linewidths of the zero-phonon line as extracted directly from optical spectra with values inferred from the first-order autocorrelation function of the photoluminescence, we quantify bounds of the homogeneous broadening and of phonon-assisted contributions. The results are discussed in terms of both the independent boson model and ab-initio results as computed from GW and Bethe-Salpeter equation approximations.

cond-mat.mes-hall↗

arXiv2025

Photoemission tomography of excitons in 2D systems: momentum-space signatures of correlated electron-hole wave functions

The momentum-space signatures of excitons can be experimentally accessed through time-resolved (pump-probe) photoelectron spectroscopy. In this work, we develop a computational framework for exciton photoemission orbital tomography (exPOT) in periodic systems, enabling the simulation and interpretation of experimental observables within many-body perturbation theory. By connecting the GW +Bethe-Salpeter equation (BSE) approach to photoemission tomography, our formalism captures exciton photoemission in periodic systems, explicitly incorporating photoemission matrix element effects induced by the light-matter interaction via the probe pulse. The correlated nature of electrons and holes introduces distinct consequences for excitonic photoemission. Using the prototypical two-dimensional material hexagonal boron nitride, we demonstrate these effects, including a dependence of the photoemission angular distribution on the pump pulse polarization. Moreover, our framework extends to excitons with finite center-of-mass momentum, making it well-suited to studying momentum-dark excitons. This provides valuable insights into the microscopic nature of excitonic phenomena in quantum materials.

cond-mat.mtrl-sci↗

arXiv2025

Strain-induced exciton mobility in layered WS2 from first principles

Exciton mobility in two-dimensional semiconductors is a key ingredient in materials-based design of optoelectronic functionalities. Monolayer transition metal dichalcogenides (TMDs) set a good test case, with tightly bound excitons and designable flexibility that offer an ideal platform for realizing strain effects on exciton energy transfer. Here, we present an ab initio study to construct strain-induced exciton energy profiles and model exciton dynamics on top of these potential surfaces. We focus on inhomogeneously-strained monolayer WS$_2$, combining excitonic band structures derived from many-body perturbation theory for a large variety of strain profiles and calculate the change in mobility characteristics using a semiclassical ballistic transport model. We connect a wealth of strain patterns to exciton drift, diffusion, and confinement. Our results point to strain-induced regimes of super-ballistic propagation and an anomalous effective diffusion, governed entirely by the strain landscape. Our results provide structure-specific understanding of ballistic strain-tunable exciton behavior, offering design principles for engineering exciton dynamics in two-dimensional materials.

cond-mat.mtrl-sci↗

arXiv2025

Data-Driven Reconstruction and Characterization of Stochastic Dynamics via Dynamical Mode Decomposition

Noise fundamentally limits the performance and predictive capabilities of classical and quantum dynamical systems by degrading stability and obscuring intrinsic dynamical characteristics. Characterizing such noise accurately is essential for enhancing measurement precision, understanding environmental interactions, and designing effective control strategies across diverse scientific and engineering domains. However, extracting the environment spectral features and associated characteristic decay or coherence times from limited and noisy datasets remains challenging. Here, we introduce a general, data-driven framework based on Dynamical Mode Decomposition (DMD) to analyze system dynamics under stochastic noise. We reinterpret DMD modes as statistical weights over an ensemble of stochastic trajectories and, via a nonlinear mapping, construct a PSD-like spectral fingerprint of the noise. This enables the identification of dominant frequency contributions in both broadband (white) and correlated ($1/f$) noise environments, as well as direct extraction of intrinsic characteristic decay times from DMD eigenvalues. To overcome instability in standard DMD-based extrapolation, we develop a constrained reconstruction method using extracted decay times as physical bounds and the learned noise as spectral weights. We demonstrate the effectiveness of this approach through simulations of quantum system dynamics subject to decoherence from noise, demonstrating its robustness and predictive capabilities and comparing it with standard methods. This methodology provides a trajectory-level framework for diagnostic and predictive analysis of stochastic processes from limited, noisy time-series data.

quant-ph↗

arXiv2025

Exciton-Exciton Annihilation Mediated by Many-Body Coulomb and Phonon Interactions: An Ab Initio Study

Exciton-exciton annihilation (EEA), in which two excitons interact to generate high-energy excitations, is an important non-radiative channel in light-induced excited-state relaxation. When efficient, this process offers an alternative route to exciton emission, potentially allowing extended energetically excited particles' lifetime and coherence. These properties are significant in designing and understanding materials-based quantum devices, particularly for low-dimensional semiconductors. Here, we present a first-principles framework to compute EEA mechanisms and rates using many-body perturbation theory within the GW and Bethe-Salpeter Equation (GW-BSE) formalism. Our method explicitly accounts for Coulomb-driven and phonon-assisted exciton-exciton scattering by explicitly evaluating the interaction channels between the constituent electrons and holes composing the BSE excitons. We apply this framework to monolayer WSe$_2$ and explore the $A$, $B$ excitation manifolds, finding picosecond-scale annihilation between bright and dark states, cross valleys, and cross peak manifolds. These channels become allowed due to scattering into free electron-hole pairs across the Brillouin zone. Our results supply new insights into non-radiative exciton relaxation mechanisms in two-dimensional materials, providing a predictive and general tool for modeling these interactions in excitonic materials.

cond-mat.mtrl-sci↗

arXiv2025

Generalized many-body exciton g-factors: magnetic hybridization and non-monotonic Rydberg series in monolayer WSe$_2$

Magneto-optics of low dimensional semiconductors, such as monolayer transition metal dichalcogenides, offers a vast playground for exploring complex quantum phenomena. However, current ab initio approaches fail to capture important experimental observations related to brightening of excitonic levels and their g-factor dependence. Here, we develop a robust and general first principles framework for many-body exciton g-factors by incorporating off-diagonal terms for the spin and orbital angular momenta of single-particle bands and many-body states for magnetic fields pointing in arbitrary spatial directions. We implement our framework using many-body perturbation theory via the GW-Bethe-Salpeter equation (BSE) and supplement our analysis with robust symmetry-based models, establishing a fruitful synergy between many-body GW-BSE and group theory. Focusing on the archetypal monolayer WSe$_2$, we accurately reproduce the known results of the low-energy excitons including the Zeeman splitting and the dark/grey exciton brightening. Furthermore, our theory naturally reveals fundamental physical mechanisms of magnetic-field hybridization of higher-energy excitons (s- and p-like) and resolves the long-standing puzzle of the experimentally measured non-monotonic Rydberg series (1s-4s) of exciton g-factors. Our framework offers a comprehensive approach to investigate, rationalize, and predict the non-trivial interplay between magnetic fields, angular momenta, and many-body exciton physics in van der Waals systems.

cond-mat.mes-hall↗

arXiv2025

Ab-initio density-matrix approach to exciton coherence: phonon scattering, Coulomb interactions and radiative recombination

Relaxation processes following light excitation in semiconductors are key in materials-based quantum technology applications. These processes are broadly studied in atomically thin transition metal dichalcogenides (TMDs), quasi-two-dimensional excitonic semiconductors in which atomistic design allows for tunable excited-state properties, such as relaxation lifetimes and photo-induced coherence. In this work, we present a density-matrix-based approach to compute exciton relaxation within a many-body ab initio perspective. We expand our previously developed Lindblad density-matrix formalism to capture multi-channel electron-hole pair relaxation processes, including phonon and Coulomb scattering as well as radiative recombination, and study their effect on the time-resolved excited-state propagation. Using monolayer MoSe$_2$ as a prototypical example, we examine many-body effects on the time-dependent dynamics of photoactive excitations, exploring how the electron-hole pair interactions are reflected in variations of the excitation energy, spectral signature, and state coherence. Our method supplies a detailed understanding of exciton relaxation mechanisms in realistic materials, offering a previously unexplored pathway to study excited-state dynamics in semiconductors from first principles.

cond-mat.mtrl-sci↗

arXiv2025

Defect-Bound Excitons in Topological Materials

Excitons, bound states of electrons and holes, are affected by the properties of the underlying band structure of a material. Defects in lattice systems may trap electronic defect states, to which an electron can be excited to form defect-bound excitons. Here, we examine the effect of band topology on excitons in systems with a single-site defect. We show that in the topological phase, when robust, in-gap, ring-shaped electronic states appear around defects, the excitons' binding energies are lowered as a result of the wide spatial profile of the defect state. In addition, the excitonic wave functions have distinct shapes that change in order with small changes in the model due to the mixed orbital character of the topological bands. Our study therefore sheds new light on the dominant mechanisms that govern the behavior of defect-bound excitons in topological materials.

cond-mat.mes-hall↗

arXiv2025

Non-adiabaticity from first principles: the exact-factorization approach for solids

The thorough treatment of electron-lattice interactions from first principles is one of the main goals in condensed matter physics. While the commonly applied adiabatic Born-Oppenheimer approximation is sufficient for describing many physical phenomena, it is limited in its ability to capture meaningful features originating from non-adiabatic coupling effects. The exact factorization method, starting from the full Hamiltonian of electrons and nuclei, provides a way to systematically account for non-adiabatic effects. This formalism was recently developed into an ab initio density functional theory framework. Within this framework we here develop a perturbative approach to the electronic states in solid state materials. We derive exact-factorization-based perturbations of the Kohn-Sham states up to second order in the nuclear displacements. These non-adiabatic features in the calculated energy and wavefunction corrections are expressed in terms of readily available density functional perturbation theory components.

cond-mat.mtrl-sci↗

arXiv2024

Spectrally resolved far-field emission pattern of single photon emitters in MoS2

We explore the optical dipole orientation of single photon emitters in monolayer MoS2 as produced by a focused helium ion beam. The single photon emitters can be understood as single sulfur vacancies. The corresponding far-field luminescence spectra reveal several photoluminescence lines below the dominating luminescence of the exciton in MoS2. These sub-bandgap emission lines were predicted by ab initio theory, but they have never been resolved in luminescence experiments because of their small amplitude. We reveal the lines by their dependence as a function of the photon energy and momentum as measured in the back focal plane of the optical circuitry. The agreement between theory and experiment suggests that the defect states interact strongly within the Brillouin zone.

cond-mat.mes-hall↗

arXiv2024

Unsupervised learning approach to quantum wavepacket dynamics from coupled temporal-spatial correlations

Understanding complex quantum dynamics in realistic materials requires insight into the underlying correlations dominating the interactions between the participating particles. Due to the wealth of information involved in these processes, applying artificial intelligence methods is compelling. Yet, unsupervised data-driven approaches typically focus on maximal variations of the individual components, rather than considering the correlations between them. Here we present an approach that recognizes correlation patterns to explore convoluted dynamical processes. Our scheme is using singular value decomposition (SVD) to extract dynamical features, unveiling the internal temporal-spatial interrelations that generate the dynamical mechanisms. We apply our approach to study light-induced wavepacket propagation in organic crystals, of interest for applications in material based quantum computing and quantum information science. We show how transformation from the input momentum and time coordinates onto a new correlation-induced coordinate space allows direct recognition of the relaxation and dephasing components dominating the dynamics and demonstrate their dependence on the initial pulse shape. Entanglement of the dynamical features is suggested as a pathway to reproduce the information required for further explainability of these mechanisms. Our method offers a route for elucidating complex dynamical processes using unsupervised AI-based analysis in multi-component systems.

cond-mat.mtrl-sci↗

arXiv2024

Designable exciton mixing through layer alignment in WS$_2$-graphene heterostructures

Optical properties of heterostructures composed of layered 2D materials, such as transition metal dichalcogenides (TMDs) and graphene, are broadly explored. Of particular interest are light-induced energy transfer mechanisms in these materials and their structural roots. Here, we use state-of-the-art first-principles calculations to study the excitonic composition and the absorption properties of WS$_2$-graphene heterostructures as a function of interlayer alignment and the local strain resulting from it. We find that Brillouin zone mismatch and the associated energy level alignment between the graphene Dirac cone and the TMD bands dictate an interplay between interlayer and intralayer excitons, mixing together in the many-body representation upon the strain-induced symmetry breaking in the interacting layers. Examining the representative cases of the 0$^\circ$ and 30$^\circ$ interlayer twist angles, we find that this exciton mixing strongly varies as a function of the relative alignment. We quantify the effect of these structural modifications on exciton charge separation between the layers and the associated graphene-induced homogeneous broadening of the absorption resonances. Our findings provide guidelines for controllable optical excitations upon interface design and shed light on the importance of many-body effects in the understanding of optical phenomena in complex heterostructures.

cond-mat.mtrl-sci↗

arXiv2023

Ultrafast Exciton Decomposition in Transition Metal Dichalcogenide Heterostructures

Heterostructures of layered transition metal dichalcogenides (TMDs) host long-lived, tunable excitons, making them intriguing candidates for material-based quantum information applications. Light absorption in these systems induces a plethora of optically excited states that hybridize both interlayer and intralayer characteristics, providing a distinctive starting point for their relaxation processes, in which the interplay between generated electron-hole pairs and their scattering with phonons play a key role. We present a first-principles theoretical approach to compute phonon-induced exciton decomposition due to rapid occupation of electron-hole pairs with finite momentum and opposite spin. Using the MoSe$_2$/WSe$_2$ heterostructure as a case study, we observe a reduction in the optical activity of bright states upon phonon scattering already in the first few femtoseconds proceeding the photoexcitation, driving exciton interlayer delocalization and subsequent variations in the exciton spin. Our results reveal an unexpected and previously unexplored starting point for exciton relaxation dynamics, suggesting increased availability for coherent interactions and non-radiative processes through ultrafast changes in exciton momentum, spatial, and spin properties upon light excitation.

cond-mat.mtrl-sci↗

arXiv2023

Phonon-driven femtosecond dynamics of excitons in crystalline pentacene from first principles

Non-radiative exciton relaxation processes are critical for energy transduction efficiencies in optoelectronic materials, but how these processes are connected to the underlying crystal structure and its associated electron, exciton, and phonon band structures is poorly understood. Here, we present a first-principles approach to explore exciton relaxation pathways in pentacene, a paradigmatic molecular crystal and optoelectronic semiconductor. We compute the momentum- and band-resolved exciton-phonon interactions, and use them to analyse key scattering channels. We find that exciton intraband transitions on femtosecond timescales leading to dark-state occupation is a dominant nonradiative relaxation channel in pentacene. We further show how the nature of real-time propagation of the exciton wavepacket is connected with the longitudinal-transverse exciton splitting, stemming from crystal anisotropy, and concomitant anisotropic exciton and phonon dispersions. Our results provide a framework for understanding time-resolved exciton propagation and energy transfer in molecular crystals and beyond.

cond-mat.mtrl-sci↗

arXiv2023

Reduced absorption due to defect-localized interlayer excitons in transition metal dichalcogenide-graphene heterostructures

Associating the presence of atomic vacancies to excited-state transport phenomena in two dimensional semiconductors is of emerging interest, and demands detailed understanding of the involved exciton transitions. Here we study the effect of such defects on the electronic and optical properties of WS$_2$-graphene and MoS$_2$-graphene van der Waals heterobilayers by employing many-body perturbation theory. We find that the combination of chalcogen defects and graphene adsorption onto the transition metal dichalcogenide layer can radically alter the optical properties of the heterobilayer, due to a combination of dielectric screening, the impact of the missing chalcogen atoms in the intralayer and interlayer optical transitions, and the different nature of each layer. By analyzing the intrinsic radiative rates of the most stable subgap excitonic features, we find that while the presence of defects introduces low-lying optical transitions, resulting in excitons with larger oscillator strength, it also decreases the optical response associated to the pristine-like transition-metal dichalcogenide intralayer excitons. Our findings relate excitonic features with interface design for defect engineering in photovoltaic and transport applications.

cond-mat.mes-hall↗

arXiv2023

Spin-defect characteristics of single sulfur vacancies in monolayer $\text{MoS}_2$

Single spin defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2 and Q*) of He-ion induced sulfur vacancies in monolayer $\text{MoS}_2$. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wavefunction extent of $\sim$ 3.5 nm. The distinct valley-Zeeman splitting in out-of-plane $B$-fields and the brightening of dark states through in-plane $B$-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab-initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

cond-mat.mes-hall↗

arXiv2022

Charge quenching at defect states in transition metal dichalcogenide-graphene van der Waals heterobilayers

We study the dynamical properties of point-like defects, represented by monoatomic chalcogen vacancies, in WS$_2$-graphene and MoS$_2$-graphene heterobilayers. Employing a multidisciplinary approach based on the combination of ab initio, model Hamiltonian and density matrix techniques, we propose a minimal interacting model that allows for the calculation of electronic transition times associated to population and depopulation of the vacancy by an additional electron. We obtain the "coarse-grained" semiclassical dynamics by means of a master equation approach and discuss the potential role of virtual charge fluctuations in the internal dynamics of impurity quasi-degenerate states. The interplay between the symmetry of the lattice and the spin degree of freedom through the spin-orbit interaction and its impact on charge quenching is studied in detail.

cond-mat.mes-hall↗