arXiv subjects

Hadas Soifer

Publications and source records attributed to Hadas Soifer.

12 recordsLinked to original sources

arXiv2025

Light-induced trion-exciton competition revealed by ultrafast photoemission

Strong Coulomb interactions in low-dimensional quantum materials give rise to emergent bound states such as excitons and trions. Trions are conventionally secondary excitations, requiring both optical excitation and charge doping. In quasi-one-dimensional Ta$_2$NiS$_5$, however, an exceptionally large binding energy exceeding the single-particle band gap stabilizes an equilibrium trion gas under surface doping alone. Here, using time- and angle-resolved photoemission spectroscopy, we show that trions can also be generated purely optically, without external charge. Following photoexcitation of pristine Ta$_2$NiS$_5$ we observe a bright, momentum-localized, in-gap feature with a slow, fluence-dependent relaxation. Rate-equation modeling identifies it as a mixed population of trions and excitons, with the trions formed via an unconventional single-particle pathway that requires no photoexcited hole. The trion-exciton composition is controlled by pump fluence, with trions dominating the late-time relaxation. In surface doped samples, the same model with unchanged rates reproduces the full dynamics, linking the light-induced trions to their equilibrium counterparts through pump-induced dissociation and recapture. These results establish trARPES as a direct probe of charged quasiparticles far from equilibrium and open routes to optical control of neutral and charged excitations in correlated materials.

cond-mat.str-el↗

arXiv2025

Trion gas on the surface of a failed excitonic insulator

Trions, three-body bound states composed of an exciton and an additional charge, are typically fragile and require external excitation to form. Here, we report the spontaneous emergence of a stable trion gas at the surface of the layered semiconductor Ta2NiS5, revealed through angle-resolved photoemission spectroscopy. We observe a sharp, highly localized in-gap feature that cannot be explained by conventional band-theory. Instead, we argue that it arises from the formation of negative trions, stabilized by surface-induced band bending and the material's quasi-one-dimensional geometry. Unlike excitons, these trions form without optical pumping and persist at equilibrium, marking a rare example of an interaction-driven surface state in a nominally conventional semiconductor. Our findings establish Ta2NiS5 as a unique platform for exploring many-body physics at surfaces and open new avenues for studying and controlling collective excitations in low-dimensional systems.

cond-mat.str-el↗

arXiv2025

Resolving the phase of a Dirac topological state via interferometric photoemission

The electronic wavefunction is at the heart of physical phenomena, defining the frontiers of quantum materials research. While the amplitude of the electron wavefunction in crystals can be measured with state-of-the-art probes in unprecedented resolution, its phase has remained largely inaccessible, obscuring rich electronic information. Here we develop a quantum-path electron interferometer based on time- and angle-resolved photoemission spectroscopy, that enables the reconstruction of phase information associated with electronic states, as encoded in the photoemission transition amplitudes - with energy and momentum resolution. We demonstrate the scheme by resolving the phase along the Dirac electronic band of a prototypical topological insulator and observe a resonance-associated phase jump as well as a momentum and phase synchronized inversion revealing the helicity of the Dirac cone. We show the interferometer can be optically controlled by the polarization of the absorbed light, allowing a differential measurement of the phase - a crucial component for extracting phase information from an interferogram. This photo-electron-interferometer provides direct experimental access to the phase of electronic transition amplitudes. Its implementation relies on experimentally accessible conditions - such as the presence of a suitable intermediate state and polarization-selective coupling - and can therefore be extended to a wide class of materials.

cond-mat.mes-hall↗

arXiv2025

Mesoscale variations of chemical and electronic landscape on the surface of Weyl semimetal Co$_3$Sn$_2$S$_2$ visualized by ARPES and XPS

The multiple crystalline terminations in magnetic Weyl semimetal Co$_3$Sn$_2$S$_2$ display distinct topological and trivial surface states, which have successfully been distinguished experimentally. However, a model of pure terminations is known to be inadequate because these surfaces exhibit a high degree of spatial heterogeneity and point disorder. Here we perform a spectromicroscopy study of the surface chemistry and surface electronic structure using photoemission measurements in combination with first-principles calculations of core levels. We identify an intermediate region with properties distinct from both the sulfur and tin terminations, and demonstrate that the spectral features in this region can be associated with a disordered termination with a varying density of surface tin vacancies. This work establishes heuristics for identifying variable surface disorder using photoemission, an important prerequisite to experimentally establishing the behavior of momentum-space topological surface features subject to variable surface disorder on a single cleave.

cond-mat.mtrl-sci↗

arXiv2025

Reexamining Circular Dichroism in Photoemission From a Topological Insulator

The orbital angular momentum (OAM) of electron states is an essential ingredient for topological and quantum geometric quantities in solids. For example, Dirac surface states with helical spin- and orbital-angular momenta are a hallmark of a 3D topological insulator. Angle-resolved photoemission spectroscopy (ARPES) with variable circular light polarization, known as circular dichroism (CD), has been assumed to be a direct probe of OAM and, by proxy, of the Berry curvature of electronic bands in energy- and momentum-space. Indeed, topological surface states have been shown to exhibit angle-dependent CD (CDAD), and more broadly, CD is often interpreted as evidence of spin-orbit coupling. Meanwhile, it is well-established that CD originates from the photoemission matrix elements, which can have extrinsic contributions related to the experimental geometry and the inherently broken inversion symmetry at the sample surface. Therefore, it is important to broadly examine CD-ARPES to determine the scenarios in which it provides a robust probe of intrinsic material physics. We performed CD-ARPES on the canonical topological insulator $\mathrm{Bi}_2\mathrm{Se}_3$ over a wide range of incident photon energies. Not only do we observe angle-dependent CD in the surface states, as expected, but we also find CD of a similar magnitude in virtually all bulk bands. Since OAM is forbidden by inversion symmetry in the bulk, we conclude this originates from symmetry-breaking in the photoemission process. Comparison with theoretical calculations supports this view and suggests that $\textit{hidden}$ OAM - localized to atomic sites within each unit cell - contributes significantly. Additional effects, including inter-atomic interference and final-state resonances, are responsible for the rapid variation of the CDAD signal with photon energy.

cond-mat.mtrl-sci↗

arXiv2025

Analysis methodology of coherent oscillations in time- and angle-resolved photoemission spectroscopy

Oscillatory signals from coherently excited phonons are regularly observed in ultrafast pump-probe experiments on condensed matter samples. Electron-phonon coupling implies that coherent phonons also modulate the electronic band structure. These oscillations can be probed with energy and momentum resolution using time- and angle-resolved photoemission spectroscopy (trARPES) which reveals the orbital dependence of the electron-phonon coupling for a specific phonon mode. However, a comprehensive analysis remains challenging when multiple coherent phonon modes couple to multiple electronic bands. Complex spectral line shapes due to strong correlations in quantum materials add to this challenge. In this work, we examine how the frequency domain representation of trARPES data facilitates a quantitative analysis of coherent oscillations of the electronic bands. We investigate the frequency domain representation of the photoemission intensity and \tred{the first moment of the energy distribution curves}. Both quantities provide complimentary information and are able to distinguish oscillations of binding energy, linewidth and intensity.We analyze a representative trARPES dataset of the transition metal dichalcogenide WTe$_2$ and construct composite spectra which intuitively illustrate how much each electronic band is affected by a specific phonon mode. We also show how a linearly chirped probe pulse can generate extrinsic artifacts that are distinct from the intrinsic coherent phonon signal.

cond-mat.mtrl-sci↗

arXiv2021

Expanding the momentum field of view in angle-resolved photoemission systems with hemispherical analyzers

In photoelectron spectroscopy, the measured electron momentum range is intrinsically related to the excitation photon energy. Low photon energies $<10$ eV are commonly encountered in laser-based photoemission and lead to a momentum range that is smaller than the Brillouin zones of most materials. This can become a limiting factor when studying condensed matter with laser-based photoemission. An additional restriction is introduced by widely used hemispherical analyzers that record only electrons photoemitted in a solid angle set by the aperture size at the analyzer entrance. Here, we present an upgrade to increase the effective solid angle that is measured with a hemispherical analyzer. We achieve this by accelerating the photoelectrons towards the analyzer with an electric field that is generated by a bias voltage on the sample. Our experimental geometry is comparable to a parallel plate capacitor and, therefore, we approximate the electric field to be uniform along the photoelectron trajectory. With this assumption, we developed an analytic, parameter-free model that relates the measured angles to the electron momenta in the solid and verify its validity by comparing with experimental results on the charge density wave material TbTe$_3$. By providing a larger field of view in momentum space, our approach using a bias potential considerably expands the flexibility of laser-based photoemission setups.

physics.ins-det↗

arXiv2021

All-optical probe of three-dimensional topological insulators based on high-harmonic generation by circularly-polarized laser fields

We report the observation of a novel nonlinear optical response from the prototypical three-dimensional topological insulator Bi$_2$Se$_3$ through the process of high-order harmonic generation. We find that the generation efficiency increases as the laser polarization is changed from linear to elliptical, and it becomes maximum for circular polarization. With the aid of a microscopic theory and a detailed analysis of the measured spectra, we reveal that such anomalous enhancement encodes the characteristic topology of the band structure that originates from the interplay of strong spin-orbit coupling and time-reversal symmetry protection. Our study reveals a new platform for chiral strong-field physics and presents a novel, contact-free, all-optical approach for the spectroscopy of topological insulators. The implications are in ultrafast probing of topological phase transitions, light-field driven dissipationless electronics, and quantum computation.

cond-mat.mes-hall↗

arXiv2018

Band resolved imaging of photocurrent in a topological insulator

We study the microscopic origins of photocurrent generation in the topological insulator Bi$_2$Se$_3$ via time- and angle-resolved photoemission spectroscopy. We image the unoccupied band structure as it evolves following a circularly polarized optical excitation and observe an asymmetric electron population in momentum space, which is the spectroscopic signature of a photocurrent. By analyzing the rise times of the population we identify which occupied and unoccupied electronic states are coupled by the optical excitation. We conclude that photocurrents can only be excited via resonant optical transitions coupling to spin-orbital textured states. Our work provides a microscopic understanding of how to control photocurrents in systems with spin-orbit coupling and broken inversion symmetry.

cond-mat.mtrl-sci↗

arXiv2016

Probe of Multi-electron Dynamics in Xenon by Caustics in High Order Harmonic Generation

We investigated the giant resonance in Xenon by high-order harmonic generation spectroscopy driven by a two-color field. The addition of a non-perturbative second harmonic component parallel to the driving field breaks the symmetry between neighboring sub-cycles resulting in the appearance of spectral caustics at two distinct cut-off energies. By controlling the phase delay between the two color components it is possible to tailor the harmonic emission in order to amplify and isolate the spectral feature of interest. In this paper we demonstrate how this control scheme can be used to investigate the role of electron correlations that give birth to the giant resonance in Xenon. The collective excitations of the giant dipole resonance in Xenon combined with the spectral manipulation associated with the two color driving field allow to see features that are normally not accessible and to obtain a quantitative good agreement between the experimental results and the theoretical predictions.

physics.atom-ph↗

arXiv2014

Studying the universality of field induced tunnel ionization times via high-order harmonic spectroscopy

High-harmonics generation spectroscopy is a promising tool for resolving electron dynamics and structure in atomic and molecular systems. This scheme, commonly described by the strong field approximation, requires a deep insight into the basic mechanism that leads to the harmonics generation. Recently, we have demonstrated the ability to resolve the first stage of the process -- field induced tunnel ionization -- by adding a weak perturbation to the strong fundamental field. Here we generalize this approach and show that the assumptions behind the strong field approximation are valid over a wide range of tunnel ionization conditions. Performing a systematic study -- modifying the fundamental wavelength, intensity and atomic system -- we observed a good agreement with quantum path analysis over a range of Keldysh parameters. The generality of this scheme opens new perspectives in high harmonics spectroscopy, holding the potential of probing large, complex molecular systems.

physics.atom-ph↗

arXiv2014

Transient grating spectroscopy of SF6 molecular vibrations

Strong field transient grating spectroscopy has shown to be a very versatile tool in time-resolved molecular spectroscopy. Here we use this technique to investigate the high-order harmonic generation from SF6 molecules vibrationally excited by impulsive stimulated Raman scattering. Transient grating spectroscopy enables us to reveal clear modulations of the harmonic emission. This heterodyne detection shows that the harmonic emission generated between 14 to 26 eV is mainly sensitive to two among the three active Raman modes in SF6, i.e. the strongest and fully symmetric nu 1-A1g mode (774 cm-1, 43 fs) and the slowest mode nu5-T2g (524 cm-1, 63 fs). A time-frequency analysis of the harmonic emission reveals additional dynamics: the strength and central frequency of the nu 1 mode oscillate with a frequency of 52 cm-1 (640 fs). This could be a signature of the vibration of dimers in the generating medium. Harmonic 11 shows a remarkable behavior, oscillating in opposite phase, both on the fast (774 cm-1) and slow (52 cm-1) timescales, which indicates a strong modulation of the recombination matrix element as a function of the nuclear geometry. These results demonstrate that the high sensitivity of high-order harmonic generation to molecularvibrations, associated to the high sensitivity of transient grating spectroscopy, make their combination a unique tool to probe vibrational dynamics.

physics.chem-ph↗