arXiv subjects

Serguei Patchkovskii

Publications and source records attributed to Serguei Patchkovskii.

At least 19 recordsLinked to original sources

arXiv2026

Disentangling the Effect of Ionic Coupling and Multiple Interfering Terms in Attosecond Molecular Interferometry

Attosecond interferometry in a two-color field is central to attosecond metrology and spectroscopy. In this technique, a photoelectron wave packet is released when a single photon from an extreme ultraviolet comb is absorbed. The wave packet then either emits or absorbs one or more near-infrared photons, leading to the formation of sidebands of the main photoelectron peaks. This picture applies well to atoms and assumes that the near-infrared laser pulse only acts on the photoelectron leaving the parent ion. The effect of the near-infrared pulse on the electronic structure of the cation is not considered, since the field usually cannot induce transitions between its electronic levels. Here, we demonstrate how dynamics induced by the near-infrared field in the cation can significantly impact the amplitude and phases of the sideband signal of the photoelectrons associated with specific dissociative channels of CO$_2$ molecules. This coupling of the near-infrared field with the molecular cation opens a third quantum pathway contributing to the signal measured in attosecond interferometry. Through angle- and energy-resolved characterization of the sideband oscillations, we observe reduction of interference amplitude over specific energy range upon angle integration. By comparison with theoretical predictions, we can isolate the contributions of specific interfering pathways to the two-color multi-pathway photoionization process. The scheme investigated in our work is general, and our observations highlight the importance of the additional pathway for accurately interpreting attosecond interferometry experiments involving molecules and more complex quantum systems.

physics.atom-ph↗

arXiv2026

Roadmap on Attosecond Science

Twenty-five years have passed since the first experimental demonstration of attosecond pulses, marking the advent of our ability to resolve and control electron motion in real time. What began as a technological breakthrough - generating the shortest flashes ever produced - has evolved into a powerful approach for probing and steering electronic dynamics in atoms, molecules, and solids. This roadmap, authored by leading experts in the field, surveys the recent rapid progress in the generation and characterization of attosecond pulses, emerging attosecond measurement and control techniques, and their expanding range of applications. It reviews current and future developments in attosecond light sources, including novel laser technologies, waveform synthesizers, new schemes for high-order harmonic generation, attosecond pulse generation at free-electron lasers, and structured light. Advances in attosecond measurement methodologies are also discussed, encompassing all-attosecond pump-probe spectroscopy, attosecond four-wave mixing, attosecond microscopy, spectroscopy with light transients, and attosecond interferometry. Furthermore, the roadmap addresses applications of attosecond spectroscopy to reveal electron dynamics in molecules and condensed matter systems from both theoretical and experimental perspectives, and highlights emerging directions at the interface with quantum optics and quantum entanglement. Overall, this work aims to serve as a comprehensive resource for navigating the evolving landscape of attosecond science.

physics.optics↗

arXiv2026

Geometric mechanisms enabling spin- and enantio-sensitive observables in one photon ionization of chiral molecules

We examine spin-resolved photoionization of randomly oriented chiral molecules via circularly polarized light, and revisit earlier predictions of Cherepkov (J. Phys. B: Atom. Mol. Phys. 16, 1543, 1983). We will show that the dynamical origin of spin- and enantio-sensitive observables arise from two intrinsic mechanisms that are quantified by two pseudovectors stemming from the geometric properties of the photoionization dipoles in spin space and in real space, and an extrinsic mechanism which is a directional bias introduced by the well-defined direction of light polarization. These mechanisms arise solely from electric dipole interactions. Consequently, this means that the ten independent parameters that was earlier predicted by Cherepkov to fully describe spin-resolved photoionization of chiral molecules can be reduced as moments of these three pseudovectors. We also find that the molecular pseudoscalars describing the spin- and enantio-sensitive components of the yield can be described by the flux of these pseudovectors through the energy shell, which changes sign upon switching enantiomers. Our results provide compact expressions for these observables which provide an intuitive picture on what determines the strength of these spin- and enantio-sensitive observables. The approach can be readily generalized to photoexcitation, multiphoton processes, and arbitrary field polarizations. Regardless of the specific driving conditions, the resulting spin- and enantio-sensitive observables are still controlled by the same three pseudovectors, underscoring their universal role as the primary generators of chirality-induced spin asymmetries, emphasizing their fundamental geometric origin and the universality of the mechanism identified here.

physics.atom-ph↗

arXiv2025

Table-top all-attosecond transient absorption spectroscopy

Attosecond transient absorption spectroscopy (ATAS) has emerged as a powerful technique within the field of attosecond science, combining extremely high temporal and excellent spectral resolution. So far, ATAS has been implemented in pump-probe experiments where an attosecond extreme-ultraviolet (XUV) pump or probe pulse was combined with a near-infrared (NIR) pulse in the femtosecond range, with the attosecond time resolution deriving from sub-cycle NIR-driven dynamics. Investigations of ultrafast electron dynamics in atoms, molecules and solids, with potential impact across physics, chemistry, and biology, would benefit significantly from the ability to perform all-attosecond transient absorption spectroscopy (AATAS). Here we demonstrate time-resolved AATAS using a table-top high-harmonic generation (HHG) source. The method is applied to investigate previously unresolved electronic coherences in Xe, revealing oscillatory valence hole motion with a 3-femtosecond period. In addition, systematic investigations of electron dynamics in Kr, Ar, and Ne are presented. Our work shows that, thanks to its broad bandwidth, high stability and easy accessibility, HHG is an ideal source for AATAS, offering the potential for replication in numerous laboratories.

physics.atom-ph↗

arXiv2025

Spin-current correlations in photoionization of chiral molecules

Chirality-induced spin selectivity (CISS) refers to phenomena where molecular chirality governs spin polarization. While symmetry simply requires chiral molecules to support spin-vector correlations, we show that CISS is fundamentally a conditioned measurement of these correlations. We illustrate this principle for spin-resolved one-photon ionization of a randomly oriented ensemble of chiral molecules. We introduce and quantify the phenomenon of enantio-sensitive locking of the photoelectron current to its spin, thereby providing a complete description of spin-conditioned photoelectron currents in one-photon ionization.

quant-ph↗

arXiv2025

Enantiosensitive molecular compass

Chirality describes the asymmetry between an object and its mirror image and underlies diverse functionalities across molecular, mesoscopic and bulk matter. A particularly intriguing example is chirality-induced spin selectivity (CISS), where chiral structures generate enantio-sensitive spin polarization. Despite extensive research, its microscopic origin and unexpectedly large magnitude remain unresolved. Here, we isolate the intrinsic coupling between chirality and spin by considering spin-resolved photoionization of randomly oriented chiral molecules under isotropic illumination. We show that electric-dipole photoionization in the presence of spin-orbit coupling generates intrinsic correlations between molecular orientation and photoelectron spin that survive complete isotropic averaging. We identify these spin-orientation correlations as the microscopic origin of CISS in photoionization and reveal their complementary manifestation: selecting the photoelectron spin orients the residual molecular ensemble, realizing spin-orientation locking, whereas selecting molecular orientation produces CISS. Both effects are governed by the same correlation strength, set by the magnitude of a molecular-frame photoionization Bloch vector that defines an enantio-sensitive molecular compass. An analogous compass emerges in photoexcitation. Our results establish spin - orientation correlations as a fundamental ingredient of chiral spin photodynamics and provide a microscopic framework for understanding and exploiting spin selectivity in chiral matter.

cond-mat.mes-hall↗

arXiv2025

High-Order Harmonic Generation in Organic Molecular Crystals

High-order harmonic generation (HHG) is a powerful tool for probing electronic structure and ultrafast dynamics in matter. Traditionally studied in atomic and molecular gases, HHG has recently been extended to condensed matter, enabling all-optical investigations of electronic and crystal structures. Here, we experimentally demonstrate HHG in a new class of materials: thin organic molecular crystals with perfectly aligned molecules, using pentacene as a model system. Organic molecular crystals, characterized by weak intermolecular coupling, flat electronic bands, and large unit cells, differ fundamentally from conventional covalent or ionic crystals and have attracted significant interest as promising candidates for organic electronics. We show that pentacene crystals endure laser intensities sufficient for efficient HHG up to the 17th order. The harmonic yield as a function of laser polarization reveals a strong dependence on intermolecular interactions, with higher harmonic orders particularly sensitive to both nearest- and next-nearest-neighbor couplings. Model calculations indicate that weaker intermolecular interactions necessitate probing with higher harmonic orders to resolve the crystal structure. These findings suggest that HHG may serve as a powerful tool for probing the electronic structure of organic molecular crystals, enhancing all-optical techniques for studying electronic properties and ultrafast dynamics in complex organic materials.

physics.optics↗

arXiv2025

In Search Of Lost Tunneling Time

The measurement of tunneling times in strong-field ionization has been the topic of much controversy in recent years, with the attoclock and Larmor clock being two of the main contenders for correctly reproducing these times. By expressing the attoclock as the weak value of temporal delay, we extend its meaning beyond the traditional setup. This allows us to calculate the attoclock time for a static one-dimensional tunneling model consisting of a binding delta potential and a constant electric field. We apply the Steinberg weak-value interpretation of the Larmor clock. Using this definition, we obtain the position-resolved time density during tunnel ionization, yielding a non-zero Larmor tunneling time. Our model allows us to derive the analogue of the position-resolved attoclock tunneling time. While non-zero at the tunnel exit, it vanishes at the detector, far away from the atom. Formally, this means that the attoclock does not measure the "local" Larmor time, but instead a "non-local" time closely related to the phase time.

quant-ph↗

arXiv2024

Generation of massively entangled bright states of light during harmonic generation in resonant media

At the fundamental level, full description of light-matter interaction requires quantum treatment of both matter and light. However, for standard light sources generating intense laser pulses carrying quadrillions of photons in a coherent state, the classical description of light during intense laser-matter interaction has been expected to be adequate. Here we show how nonlinear optical response of matter can be controlled to generate dramatic deviations from this standard picture, including generation of several squeezed and entangled harmonics of the incident laser light. In particular, such non-trivial quantum states of harmonics are generated as soon as one of the harmonics induces a transition between different laser-dressed states of the material system. Such transitions generate an entangled light-matter wavefunction, which can generate quantum states of harmonics even in the absence of a quantum driving field or material correlations. In turn, entanglement of the material system with a single harmonic generates and controls entanglement between different harmonics. Hence, nonlinear media that are near-resonant with at least one of the harmonics appear to be quite attractive for controlled generation of massively entangled quantum states of light. Our analysis opens remarkable opportunities at the interface of attosecond physics and quantum optics, with implications for quantum information science.

quant-ph↗

arXiv2024

Spin-Polarized Photoelectrons in the Vicinity of Spectral Features

It has been shown by Fano (1969) https://doi.org/10.1103/PhysRev.178.131 that photoionization of a cæsium atom by a laser pulse tuned to the vicinity of a Cooper minimum generates spin-polarized electrons. Here we show that while photoionization of rare gases does not provide large spin polarization in the vicinity of the Cooper minimum, the Fano resonances yield much higher overall spin polarization ($\ge40\%$). The spin polarization increases in angle-resolved photoelectron spectra, and reaches $100\%$ when measured in coincidence with the photoion. We provide a general framework for achieving spin polarization in photoionization irrespective of the ionization regime.

physics.atom-ph↗

arXiv2024

High-energy, few-cycle light pulses tunable across the vacuum ultraviolet

In the last few decades the development of ultrafast lasers has revolutionized our ability to gain insight into light-matter interactions. The appearance of few-cycle light sources available from the visible to the mid-infrared spectral range and the development of attosecond extreme ultraviolet and x-ray technologies provide for the first time the possibility to directly observe and control ultrafast electron dynamics in matter on their natural time scale. However, few-fs sources have hardly been available in the deep ultraviolet (DUV; 4-6 eV, 300-200 nm) and are unavailable in the vacuum ultraviolet (VUV; 6-12 eV, 200-100 nm) spectral range, corresponding to the photon energies required for valence excitation of atoms and molecules. Here, we generate VUV pulses with $μ$J energy tunable between 160 and 190 nm via resonant dispersive wave emission during soliton self-compression in a capillary. We fully characterize the pulses in situ using frequency-resolved optical gating based on two-photon photoionization in noble gases. The measurements reveal that in most of the cases the pulses are shorter than 3 fs. These findings unlock the potential to investigate ultrafast electron dynamics with a time-resolution that has been hitherto inaccessible when using VUV pulses.

physics.optics↗

arXiv2024

Bidirectional cascaded superfluorescent lasing in air enabled by resonant third harmonic photon exchange from nitrogen to argon

Cavity-free lasing in atmospheric air has stimulated intense research towards fundamental understanding of underlying physical mechanisms. In this Letter, we identify a new mechanism -- third harmonic photon mediated resonant energy transfer pathway leading to population inversion in argon via initial three-photon excitation of nitrogen molecules irradiated by intense 261 nm pulses -- that enables bidirectional two-color cascaded lasing in atmospheric air. By making pump-probe measurements, we conclusively show that such cascaded lasing results from superfluorescence (SF) rather than amplified spontaneous emission (ASE). Such cascaded lasing with the capability of producing bidirectional multicolor coherent pulses opens additional possibilities for remote sensing applications.

physics.optics↗

arXiv2023

Control of Spin Polarization through Recollisions

Using only linearly polarized light, we study the possibility of generating spin-polarized photoelectrons from xenon atoms. No net spin polarization is possible, since the xenon ground state is spin-less, but when the photoelectron are measured in coincidence with the residual ion, spin polarization emerges. Furthermore, we show that ultrafast dynamics of the recolliding photoelectrons contribute to an apparent flipping of the spin of the photoelectron, a process that has been completely neglected so far in all analyses of recollision-based processes. We link this phenomenon to the ``spin--orbit clock'' of the remaining ion. These effects arise already in dipole approximation.

physics.atom-ph↗

arXiv2023

Role of Spin-Orbit Coupling in High-order Harmonic Generation Revealed by Super-Cycle Rydberg Trajectories

High-harmonic generation is typically thought of as a sub-laser-cycle process, with the electron's excursion in the continuum lasting a fraction of the optical cycle. However, it was recently suggested that long-lived Rydberg states can play a particularly important role in atoms driven by the combination of the counter-rotating circularly polarized fundamental light field and its second harmonic. Here we report direct experimental evidence of long and stable Rydberg trajectories contributing to high-harmonic generation. We confirm their effect on the harmonic emission via Time-Dependent Schr{ö}dinger Equation simulations and track their dynamics inside the laser pulse using the spin-orbit evolution in the ionic core, utilizing the spin-orbit Larmor clock. Our observations contrast sharply with the general view that long-lived Rydberg orbits should generate negligible contribution to the macroscopic far-field high harmonic response of the medium. Indeed, we show how and why radiation from such states can lead to well collimated macroscopic signal in the far field.

physics.atom-ph↗

arXiv2023

Isotopic effects in molecular attosecond photoelectron interferometry

Isotopic substitution in molecular systems can affect fundamental molecular properties including the energy position and spacing of electronic, vibrational and rotational levels, thus modifying the dynamics associated to their coherent superposition. In extreme ultraviolet spectroscopy, the photoelectron leaving the molecule after the absorption of a single photon can trigger an ultrafast nuclear motion in the cation, which can lead, eventually, to molecular fragmentation. This dynamics depends on the mass of the constituents of the cation, thus showing, in general, a significant isotopic dependence. In time-resolved attosecond photoelectron interferometry, the absorption of the extreme ultraviolet photon is accompanied by the exchange of an additional quantum of energy (typically in the infrared spectral range) with the photoelectron-photoion system, offering the opportunity to investigate in time the influence of isotopic substitution on the characteristics of the photoionisation dynamics. Here we show that attosecond photoelectron interferometry is sensitive to isotopic substitution by investigating the two-color photoionisation spectra measured in a mixture of methane (CH$_4$) and deuteromethane (CD$_4$). The isotopic dependence manifests itself in the modification of the amplitude and contrast of the oscillations of the photoelectron peaks generated in the two-color field with the two isotopologues. The observed effects are interpreted considering the differences in the time evolution of the nuclear autocorrelation functions in the two molecules.

physics.atom-ph↗

arXiv2022

Imprinting chirality on atoms using synthetic chiral light fields

Atoms are usually thought of as achiral objects. However, one can construct superpositions of atomic states that are chiral [1]. Here we show how to excite such superpositions with tailored light fields both in the weak-field and strong-field regimes, using realistic laser parameters. First, we use time-dependent Schrodinger equation (TDSE) simulations to demonstrate the creation of a time-dependent bound chiral wavepacket in sodium atoms. Second, we show how the time-dependent handedness of this wavepacket can be probed by photoelectron circular dichroism, in spite of the central symmetry of the core potential. Third, we use TDSE simulations to show how chirality can be directly imprinted on a photoelectron wavepacket created by strong-field ionization and introduce an unambigous chiral measure that allows us to characterize its handedness.

physics.atom-ph↗

arXiv2022

Rydberg Atomic Antenna in Strongly Driven Multi-Electron Atoms

We study the role of intermediate excitations of Rydberg states as an example of Kuchiev's "atomic antenna" in above-threshold ionization of xenon, in particular their effect on the coherence between the spin-orbit-split states of the ion. We focus on the case of a laser frequency close to resonant with the spin-orbit splitting, where a symmetry (parity) argument would preclude any coherence being directly generated by strong-field ionization. Using ab initio simulations of coupled multielectron spin-orbit dynamics in strong laser fields, we show how field-driven rescattering of the trapped Rydberg electrons introduces efficient coupling between the spin-orbit-split channels, leading to substantial coherences, exceeding 10 % for some photon energies.

physics.atom-ph↗

arXiv2022

Theory of nuclear motion in RABBITT spectra

Reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) is a powerful photoelectron spectroscopy, offering direct access to internal dynamics of the target. It is being increasingly applied to molecular systems, but a general, computationally tractable theory of RABBITT spectra in molecules has so far been lacking. We show that under quite general assumptions, RABBITT spectra in molecules can be expressed as a convolution of the vibronic cross-correlation functions and two-electron photoionization matrix elements. We specialize the general expressions to the commonly-encountered special cases. We expect our theory to enable accurate modeling and interpretation of molecular RABBITT spectra in most medium-sized molecules.

physics.chem-ph↗