arXiv subjects

Anh-Thu Le

Publications and source records attributed to Anh-Thu Le.

At least 19 recordsLinked to original sources

arXiv2026

Strong-field Herman-Kluk propagator method for high-harmonic generation in molecules

We extend our recently developed semiclassical strong-field Herman-Kluk (SFHK) propagator method to calculate high-order harmonic generation (HHG) in diatomic molecules driven by few-cycle intense laser fields. On the example of applications to H2 and N2, we show that our method, based on a combination of the Herman-Kluk propagator and the strong-field approximation, can provide very accurate results for both HHG yield and phase, nearly identical to those from the exact numerical solutions of the time-dependent Schrodinger equation. To compare with experimental measurements, averaging over molecular orientations must be performed. Here we demonstrate a distinct and powerful advantage of the SFHK, as its Monte Carlo sampling for the integration over the alignment distribution can be efficiently combined with the integration over the initial momentum distributions of electron wave-packet right after the tunnel exit. Therefore, the total number of trajectories used for the alignment-averaged HHG spectrum does not increase much compared to that for a single fixed alignment. Similar to atomic targets, the main computational task in the SFHK is to solve the classical Hamiltonian equations for the active electron in the combined electron-target ion potential and electron-laser interaction. The motion of the center of each electron wave packet in the continuum, represented by a coherent state, is governed by an independent classical trajectory so that the computation can be parallelized very efficiently.

physics.atom-ph↗

arXiv2026

Fact-Checking at Scale: Multimodal AI for Authenticity and Context Verification in Online Media

The proliferation of multimedia content on social media platforms has dramatically transformed how information is consumed and disseminated. While this shift enables real-time coverage of global events, it also facilitates the rapid spread of misinformation and disinformation, especially during crises such as wars, natural disasters, or elections. The rise of synthetic media and the reuse of authentic content in misleading contexts have intensified the need for robust multimedia verification tools. In this paper, we present a comprehensive system developed for the ACM Multimedia 2025 Grand Challenge on Multimedia Verification. Our system assesses the authenticity and contextual accuracy of multimedia content in multilingual settings and generates both expert-oriented verification reports and accessible summaries for the general public. We introduce a unified verification pipeline that integrates visual forensics, textual analysis, and multimodal reasoning, and propose a hybrid approach to detect out-of-context (OOC) media through semantic similarity, temporal alignment, and geolocation cues. Extensive evaluations on the Grand Challenge benchmark demonstrate the system's effectiveness across diverse real-world scenarios. Our contributions advance the state of the art in multimedia verification and offer practical tools for journalists, fact-checkers, and researchers confronting information integrity challenges in the digital age.

cs.MM↗

arXiv2026

Spectral properties of high-order harmonic radiation enhanced by XUV-driven electron-hole dynamics

We analyze the spectral properties of high-order harmonic radiation with photon energies extending beyond the regular cutoff energy in standard high-order harmonic generation. The extension of the regular harmonic cutoff results from infrared (IR)-driven recombination of valence photoelectrons into a cationic core hole created by extreme-ultraviolet (XUV) excitation of inner-shell electrons into the transient valence hole in a combined XUV+IR configuration [Buth et al., Opt. Lett. 36, 3530 (2011)]. We show that the microscopic dipole phase at the extended harmonic frequencies is sensitive to the relative IR-XUV delay and IR intensity, whereas the corresponding signal intensity drops significantly for chirped XUV pulses with poor temporal coherence. We discuss the impact of such sensitivity on the macroscopic harmonic radiation, whereby decoherence among the dipole emitters may lead to further signal suppression.

physics.atom-ph↗

arXiv2026

Highly accurate semiclassical strong-field Herman-Kluk propagator method for high-harmonic generation

We extend our recently developed semiclassical strong-field Herman-Kluk propagator (SFHK) method to calculate high-order harmonic generation (HHG) for atoms in intense lasers. We show that our method, based on a combination of the Herman-Kluk propagator and the strong-field approximation, can provide highly accurate results for both HHG yield and phase, nearly identical to those from the exact numerical solutions of the time-dependent Schrödinger equation. We provide detailed analyses of our method and its applications to the HHG process, particularly the recombination time. The main computational task in this method is to solve the classical Newton equations for the active electron in the combined atomic potential and laser-electron interaction. The motion of the centers of the electron wave packets, modeled by coherent states, is governed by independent classical trajectories so that the computation can therefore be parallelized very efficiently.

physics.atom-ph↗

arXiv2026

Single photon zeptosecond interferometry

We demonstrate the generation of a train of attosecond XUV pulses that are in a superposition of wavefront states. Such superposition yields a high precision, self-referencing, common path XUV interferometer setup to produce pairs of spatially separated and independently controllable XUV pulses that are locked in phase and time with a temporal jitter of 3.5 zs (zs = zeptoseconds = $10^{-21}$). In our approach, we can independently control the relative phase/delay of the two optical beams with a resolution of 52 zs. Since the jitter is on the order of the Compton time scale, we explore the level of correlation between the non-local photons by comparing different spatial mode superpositions. Further, thanks to the stability of the interferometer we can retrieve the interference pattern through photon counting. Through post-selection of different particle events we can analyze one, two or more photon events. We argue that this zeptosecond level of temporal precision will open the door for new dynamical QED tests at lower intensities while photon counting experiments can also have an impact on the emerging field of quantum light in strong fields. We also discuss the potential impact on other areas, such as time-dependent QED, imaging, measurements of non-locality, and molecular quantum tomography.

physics.optics↗

arXiv2025

Delay in electronic vortex states created by multiphoton ionization with single elliptically polarized laser pulses

We show experimentally and theoretically that vortex-shaped structures in the photoelectron momentum distribution can be observed for atoms interacting with a single intense elliptically polarized laser pulse. Our analysis reveals that these spiral structures are the result of destructive interference of two dominant photoelectron vortex states, which are released into the continuum by strong-field ionization. An electron born into one of those states is temporarily delayed near the atomic core by the combined atomic and laser potential, leading to fast changes in the phase delay with energy for photoelectrons in these vortex states. Our results open the door to studying electron dynamics of vortex states in strong-field ionization.

physics.atom-ph↗

arXiv2025

Strong-Field Photoelectron Interferometry with Near-Single-Cycle Yb Lasers

The concept of using photoelectron interferometry in short laser fields to probe electron dynamics and target structures was introduced more than two decades ago. However, the quality of experimental data has remained insufficient for quantitative analysis, largely due to the instability of few-cycle Ti:Sa laser pulses, the current workhorse of short pulses. Here, we report the first systematic strong-field ionization experiments performed with industrial-grade, carrier-envelope-phase (CEP) stabilized, near-single-cycle Yb lasers. By measuring photoelectron momentum distributions in the direct-ionization regime, we show that single-cycle cosine-shaped pulses can separate and enhance both spider-leg and fishbone holographic structures. The spider-leg structure enables extraction of the electron scattering phase from the Ar atomic potential-information typically accessible only through attosecond metrology, while the fishbone structure reveals the orbital-parity contrast between Ar atoms and nitrogen molecules. Our measurements are quantitatively reproduced by both semiclassical Herman-Kluk-propagator and \textit{ab initio} simulations, paving the way for precision studies of electron-molecule scattering with widely accessible industrial-grade lasers.

physics.atom-ph↗

arXiv2024

Coherent postionization dynamics of molecules based on adiabatic strong-field approximation

Taking N2 and O2 as examples, we theoretically study the post-ionization dynamics of molecules in strong laser fields using a density matrix method for open systems, focusing on the effect of ionization-produced coherence on the dynamics of residual ions. We introduce the adiabatic strong-field approximation (ASFA) method to predict the coherences between ionic states resulting from multiorbital strong-field ionizations. Compared with the standard SFA, the ASFA method can be applied across a wide range of laser intensities due to the consideration of orbital distortion effects. Based on the ASFA, it is found that there are obvious coherences between ionic states in residual molecular ions. These coherences significantly influence the transitions between ionic states, which finally change the post-ionization dynamics of molecular ions. Our findings reveal the importance of the ionization-produced coherences in modulating post-ionization molecular dynamics.

physics.atom-ph↗

arXiv2024

Quantum pathways interference in laser-induced electron diffraction revealed by a semiclassical method

We develop a novel method for strong-laser-field physics based on the combination of the semiclassical Herman-Kluk propagator and the strong-field approximation and demonstrate its high accuracy on the calculations of photoelectron momentum distribution (PMD) for atoms and molecules in intense lasers. For rescattered electrons, we show that for a given time that electron tunnels to the continuum, there are typically multiple trajectories that lead to the same final momentum in the high-energy region. These trajectories start with slightly different initial transverse momenta and carry different phases giving rise to the interference structures in the PMD, which can also be associated with the laser-free electron-ion differential cross section. This is in contrast to the well-known long and short trajectories, which result in different interference patterns. Our results can be used to extend current capabilities of the laser-induced electron diffraction and other ultrafast imaging and strong-field spectroscopic techniques.

physics.atom-ph↗

arXiv2024

Symmetries in 3D photoelectron momentum spectroscopy as precursory methods for dichroic and enantiosensitive measurements

3D photoelectron angular distributions (PADs) are measured from an atomic target ionized by ultrafast, elliptical fields of opposite handedness. Comparing these PADs to one another and to numeric simulations, a difficult to avoid systematic error in their orientation is identified and subsequently corrected by imposing the dichroic symmetry by which they are necessarily related. We show that this correction can be directly applied to molecular targets in the same fields. This paves the way for measurement of enantiosensitive information which has yet to be accessed experimentally.

physics.atom-ph↗

arXiv2020

Laser-induced electron diffraction of the ultrafast umbrella motion in ammonia

Visualizing molecular transformations in real-time requires a structural retrieval method with Ångström spatial and femtosecond temporal atomic resolution. Imaging of hydrogen-containing molecules additionally requires an imaging method that is sensitive to the atomic positions of hydrogen nuclei, with most methods possessing relatively low sensitivity to hydrogen scattering. Laser-induced electron diffraction (LIED) is a table top technique that can image ultrafast structural changes of gas-phase polyatomic molecules with sub-Ångström and femtosecond spatiotemporal resolution together with relatively high sensitivity to hydrogen scattering. Here, we image the umbrella motion of an isolated ammonia molecule (NH$_3$) following its strong field ionization. Upon ionization of a neutral ammonia molecule, the ammonia cation (NH$_3^+$) undergoes an ultrafast geometrical transformation from a pyramidal ($Φ_{HNH} = 107 ^\circ$) to planar ($Φ_{HNH}=120^\circ$) structure in approximately 8 femtoseconds. Using LIED, we retrieve a near-planar ($Φ_{HNH}=117 \pm 5^\circ$) field-dressed NH$_3^+$ molecular structure $7.8-9.8$ femtoseconds after ionization. Our measured field-dressed NH$_3^+$ structure is in excellent agreement with our calculated equilibrium field dressed structure using quantum chemical ab initio calculations.

physics.chem-ph↗

arXiv2019

Factorization of high-harmonic generation yields in impurity-doped materials

We present a theoretical investigation of high-harmonic generation (HHG) from impurity-doped materials using the time-dependent Schrödinger equation (TDSE) approach. We demonstrate the factorization of HHG yields as a product of an electron wave packet and the recombination cross section, in analogy to HHG from atoms and molecules in the gas phase. Furthermore, we show that the quantitative rescattering model based on this factorization accurately reproduces the TDSE results. This opens up new possibilities to study impurities in materials using the available techniques from strong-field physics.

physics.optics↗

arXiv2019

Imaging an isolated water molecule using a single electron wave packet

Observing changes in molecular structure requires atomic-scale Ångstrom and femtosecond spatio-temporal resolution. We use the Fourier transform (FT) variant of laser-induced electron diffraction (LIED), FT-LIED, to directly retrieve the molecular structure of ${\rm H_2O^+}$ with picometre and femtosecond resolution without a priori knowledge of the molecular structure nor the use of retrieval algorithms or ab initio calculations. We identify a symmetrically stretched ${\rm H_2O^+}$ field-dressed structure that is most likely in the ground electronic state. We subsequently study the nuclear response of an isolated water molecule to an external laser field at four different field strengths. We show that upon increasing the laser field strength from 2.5 to 3.8 V/Å, the O-H bond is further stretched and the molecule slightly bends. The observed ultrafast structural changes lead to an increase in the dipole moment of water and, in turn, a stronger dipole interaction between the nuclear framework of the molecule and the intense laser field. Our results provide important insights into the coupling of the nuclear framework to a laser field as the molecular geometry of ${\rm H_2O^+}$ is altered in the presence of an external field.

physics.chem-ph↗

arXiv2019

Imaging the Renner-Teller effect using laser-induced electron diffraction

Structural information on electronically excited neutral molecules can be indirectly retrieved, largely through pump-probe and rotational spectroscopy measurements with the aid of calculations. Here, we demonstrate the direct structural retrieval of neutral carbonyl disulfide (CS$_2$) in the B$^1$B$_2$ excited electronic state using laser-induced electron diffraction (LIED). We unambiguously identify the ultrafast symmetric stretching and bending of the field-dressed neutral CS$_2$ molecule with combined picometer and attosecond resolution using intrapulse pump-probe excitation and measurement. We invoke the Renner-Teller effect to populate the B$^1$B$_2$ excited state in neutral CS$_2$, leading to bending and stretching of the molecule. Our results demonstrate the sensitivity of LIED in retrieving the geometric structure of CS$_2$, which is known to appear as a two-center scatterer.

physics.chem-ph↗

arXiv2016

Orientation Resolution through Rotational Coherence Spectroscopy

The rich information content of measurements in the molecular frame rather than the laboratory frame has motivated the development of several methods for aligning gas phase molecules in space. Even so, for asymmetric tops the problem of making molecular frame measurements remains challenging due to its inherently multi-dimensional nature. In this Letter we present a method, based on the analysis of observables measured from rotational wavepackets, that does not require either 3D alignment or coincident momentum measurements to access the molecular frame. As an application we describe the first fully-orientation-resolved measurements of strong-field ionization and dissociation of an asymmetric top (ethylene).

physics.atom-ph↗

arXiv2015

Imaging an aligned polyatomic molecule with laser-induced electron diffraction

Laser-induced electron diffraction is an evolving tabletop method, which aims to image ultrafast structural changes in gas-phase polyatomic molecules with sub-Ångström spatial and femtosecond temporal resolution. Here, we provide the general foundation for the retrieval of multiple bond lengths from a polyatomic molecule by simultaneously measuring the C-C and C-H bond lengths in aligned acetylene. Our approach takes the method beyond the hitherto achieved imaging of simple diatomic molecules and is based upon the combination of a 160 kHz mid-IR few-cycle laser source with full three-dimensional electron-ion coincidence detection. Our technique provides an accessible and robust route towards imaging ultrafast processes in complex gas phase molecules with atto- to femto-second temporal resolution.

physics.atom-ph↗

arXiv2011

Intensity dependence of multiple orbital contributions and shape resonance in high-order harmonic generation of aligned N$_{2}$ molecules}

We report measurements and theoretical simulations of high-order harmonic generation (HHG) in aligned N$_2$ molecules using a 1200-nm intense laser field when the generating pulse is perpendicular to the aligning one. With increasing laser intensity, the minimum in the HHG spectra first shifts its position and then disappears. Theoretical simulations including the macroscopic propagation effects in the medium reproduce these observations and the disappearance of the minimum is attributed to the additional contribution of HHG from inner orbitals. We also predict that the well-known shape resonance in the photoionization spectra of N$_2$ should exist in the HHG spectra. It is most clearly seen when the generating laser is parallel to the aligning one, and disappears gradually as the angle between the two lasers increases. No clear evidence of this shape resonance has been reported so far when using lasers with different wavelengths. Further experimentation is needed to draw conclusions.

physics.optics↗

arXiv2011

Influence of gas pressure on high-order harmonic generation of Ar and Ne

We study the effect of gas pressure on the generation of high-order harmonics where harmonics due to individual atoms are calculated using the recently developed quantitative rescattering theory, and the propagation of the laser and harmonics in the medium is calculated by solving the Maxwell's wave equation. We illustrate that the simulated spectra are very sensitive to the laser focusing conditions at high laser intensity and high pressure since the fundamental laser field is severely reshaped during the propagation. By comparing the simulated results with several experiments we show that the pressure dependence can be qualitatively explained. The lack of quantitative agreement is tentatively attributed to the failure of the complete knowledge of the experimental conditions.

physics.atom-ph↗