arXiv subjects

Alexei N. Grum-Grzhimailo

Publications and source records attributed to Alexei N. Grum-Grzhimailo.

14 recordsLinked to original sources

arXiv2026

General properties of the RABBITT at parity mixing conditions

Parity mixing in photoionization, i.e. when emitted electrons have different parities but the same energy, causes interference observable only in angle-resolved measurements. The interference typically manifests as a symmetry violation in the photoelectron angular distributions. The traditional, based on HHG, RABBITT scheme with high-order harmonics separated by twice the seed field energy, precludes parity mixing. On the contrary, a free-electron laser provides a possibility to generate even harmonics. Using triple the fundamental frequency as a seed, one obtains a comb of alternating even and odd harmonics, separated by three times the initial frequency [Nature 578, 386-391 (2020)] (2-SB RABBITT). In this setup, there are two sidebands between the main photoelectron lines, versus one in the traditional scheme. In the paper, we examine the general properties of a two-sideband scheme and analyze the symmetry breakdown of photoelectron angular distributions for various polarization geometries of the incident pulse. We found a crucial difference in symmetries between 2-SB RABBITT and other photoionization schemes with parity mixing. Illustrative calculations are carried out for neon with pulse parameters typical for modern facilities. The possibility to reconstruct the temporal profile of the pulse from the angle-resolved measurements is discussed.

physics.atom-ph↗

arXiv2026

Dynamics of electromagnetically induced water molecule fragmentation

The development of intense high-energy radiation sources and the improvement of techniques for detecting charged fragments have made possible experiments on multiple ionization of a molecule with registration of the momentum and charge of dissociation products in coincidence. This technique allows to determine (`fix') a molecular geometry at the time of fragmentation and called fixed-in-space molecule. In this work, the dynamics the water molecule dissociation fragments resulting from interaction with intense X-ray radiation has been studied. The charge distribution of oxygen ions was calculated, Newton diagrams were constructed for fragments - protons and the oxygen ion - for various charge states of the latter, and the released kinetic energy was evaluated. Calculations were performed using the [1]code for parameters close to [2]. The predictions for the different pulse parameters are done.

physics.atom-ph↗

arXiv2025

Dichroic Electron Emission Patterns from Oriented Helium Ions

We report a joint experimental and theoretical study using a combination of polarization-controlled free-electron-laser (FEL) and near-infra\-red (NIR) pulses in a synchronized two-color photo\-ionization scheme. Excited He$^+$ ions, created by extreme ultraviolet (XUV) circularly polarized radiation from the XUV-FEL FERMI in the oriented $3p\, (m\!=\!+1)$ state, are exposed to circularly polarized 784-nm NIR radiation with peak intensities from $10^{12}\,\rm W/cm^2$ to $\rm 10^{13}\,W/cm^2$. The angular distribution of the ejected electrons exhibit a strong dichroism depending on the NIR intensity. While the co-rotating case is defined by a single path, for the counter-rotating case, there are two dominant pathways whose relative strength and phase difference are determined.

physics.atom-ph↗

arXiv2024

The Advantages of Polarization Control in RABBITT

The RABBITT setup is theoretically studied for various combinations of XUV and IR field components polarization: 'linear+linear', `linear+circular' with crossed propagation directions, and `circular+circular' with parallel propagation directions. The general properties of photoelectron angular distributions and their responses to the variation of the IR pulse delay are studied. Numerical simulations are performed for the neon valence shell ionization into the region of structureless continuum using two approaches based on time dependent perturbation theory and solution of rate equations. To distinguish between "geometrical" governed by fields' polarization and spectroscopic features, additional analysis for the case of $s$-shell ionization is presented.

physics.atom-ph↗

arXiv2024

Circular Dichroism in Multiphoton Ionization of Resonantly Excited Helium Ions near Channel Closing

The circular dichroism (CD) of photoelectrons generated by near-infrared (NIR) laser pulses using multiphoton ionization of excited He$^+$ ions in the 3p(m=+1) state. The ions were prepared by circularly polarized extreme ultraviolet (XUV) pulses. For circularly polarized NIR pulses co- and counter-rotating relative to the polarization of the XUV pulse, a complex variation of the CD is observed as a result of intensity- and polarization-dependent Freeman resonances, with and without additional dichroic AC-Stark shifts. The experimental results are compared with numerical solutions of the time-dependent Schrödinger equation to identify and interpret the pronounced variation of the experimentally observed CD.

physics.atom-ph↗

arXiv2023

Vector parameters in atomic ionization by twisted light: polarization of electron and residual ion

The electron and ion properties observed in a photoionization inherit a symmetry properties of both a target and a radiation. Introducing a symmetry breaking in a photoionization process one can expect to observe a noticeable variation of the vector correlation parameters of either outgoing photoelectron or a residual ion. One of the ways to violate symmetry is to irradiate a matter by the twisted radiation which involves an additional screw. In the paper we present the extension of the approach developed in [Phys. Rev. A 108, 023117 (2023)] for the photoelectron angular distribution to the other vector correlation parameters, exactly photoelectron spin polarization, orientation and alignment of the residual ion. Usually two conditions are needed to produce polarized photoelectrons: a system possesses a helix and a noticeable spin-orbital interaction. In the paper we investigate if a twisted light brings an additional helicity to a system. As an illustrative example we consider ionization of valence $4p$-shell of atomic krypton by circularly and linearly polarized Bessel light. The photoelectron spin components are analyzed as a function of the cone angle of the twisted radiation.

physics.atom-ph↗

arXiv2023

Angular distribution of photoelectrons generated in atomic ionization by twisted radiation

Until recently, theoretical and experimental studies of photoelectron angular distributions (PADs) including non-dipole effects in atomic photo\-ionization have been performed mainly for the conventional plane-wave radiation. One can expect, however, that the non-dipole contributions to the angular- and polarization-resolved photo\-ionization properties are enhanced if an atomic target is exposed to twisted light. The purpose of the present study is to develop a theory for PADs to the case of twisted light, especially for many-electron atoms. The theoretical analysis is performed for the experimentally relevant case of macroscopic atomic targets, i.e., when the cross-sectional area of the target is larger than the characteristic transversal size of the twisted beam. For such a scenario, we derive expressions for the angular distribution of the emitted photoelectrons under the influence of twisted Bessel beams. As an illustrative example, we consider helium photo\-ionization in the region of the lowest dipole $2s2p\,[{^1P}_1]$ and quadrupole $2p^2\,[{^1D}_2]$ autoionization resonances. A noticeable variation of the PAD caused by changing the parameters of the twisted light is predicted.

physics.atom-ph↗

arXiv2022

Evolution of the ionic polarization in multiple sequential ionization: general equations and an illustrative example

The modern Free-Electron-Lasers generate a highly intense polarized radiation which initiate a sequence of ionization and decay events. Their probability depends on the polarization of each state as function of time. Its complete accounting is limited by the fact that a state can be formed in various ways. Here we present the equivalent of rate equations for population that completely accounts polarization of radiation and formulated in terms of the statistical tensors. To illustrate our approach we theoretically consider sequential photoionization of krypton by an intense extreme ultraviolet femtosecond pulse for the photon energies below the 3d-shell excitation threshold. The calculations of the ion yields, photoelectron spectra and ionic polarization for various photon fluence are presented and role of polarization is discussed.

physics.atom-ph↗

arXiv2020

Attosecond Pulse-shaping using a seeded free-electron laser

Attosecond pulses are fundamental for the investigation of valence and core-electron dynamics on their natural timescale. At present the reproducible generation and characterisation of attosecond waveforms has been demonstrated only through the process of high-order harmonic generation. Several methods for the shaping of attosecond waveforms have been proposed, including metallic filters, multilayer mirrors and manipulation of the driving field. However, none of these approaches allow for the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free Electron Lasers, on the contrary, deliver femtosecond, extreme ultraviolet and X-ray pulses with energies ranging from tens of $\mathrmμ$J to a few mJ. Recent experiments have shown that they can generate sub-fs spikes, but with temporal characteristics that change shot-to-shot. Here we show the first demonstration of reproducible generation of high energy ($\mathrmμ$J level) attosecond waveforms using a seeded Free Electron Laser. We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with a novel approach for its temporal reconstruction. The results presented here open the way to perform attosecond time-resolved experiments with Free Electron Lasers.

physics.optics↗

arXiv2020

Atomic, molecular and optical physics applications of longitudinally coherent and narrow bandwidth Free-Electron Lasers

Short wavelength Free-Electron Lasers (FELs) are the newest light sources available to scientists to probe a wide range of phenomena, with chemical, physical and biological applications, using soft and hard X-rays. These sources include the currently most powerful light sources in the world (hard X-ray sources) and are characterised by extremely high powers and high transverse coherence, but the first FELs had reduced longitudinal coherence. Now it is possible to achieve good longitudinal coherence (narrow bandwidth in the frequency domain) and here we discuss and illustrate a range of experiments utilising this property, and their underlying physics. The primary applications are those which require high resolution (for example resonant experiments), or temporal coherence (for example coherent control experiments). The currently available light sources extend the vast range of laboratory laser techniques to short wavelengths.

physics.atom-ph↗

arXiv2020

A new method for measuring angle-resolved phases in photoemission

Quantum mechanically, photoionization can be fully described by the complex photoionization amplitudes that describe the transition between the ground state and the continuum state. Knowledge of the value of the phase of these amplitudes has been a central interest in photoionization studies and newly developing attosecond science, since the phase can reveal important information about phenomena such as electron correlation. We present a new attosecond-precision interferometric method of angle-resolved measurement for the phase of the photoionization amplitudes, using two phase-locked Extreme Ultraviolet pulses of frequency $ω$ and $2ω$, from a Free-Electron Laser. Phase differences $Δ\tilde η$ between one- and two-photon ionization channels, averaged over multiple wave packets, are extracted for neon $2p$ electrons as a function of emission angle at photoelectron energies 7.9, 10.2, and 16.6 eV. $Δ\tilde η$ is nearly constant for emission parallel to the electric vector but increases at 10.2 eV for emission perpendicular to the electric vector. We model our observations with both perturbation and \textit{ab initio} theory, and find excellent agreement. In the existing method for attosecond measurement, Reconstruction of Attosecond Beating By Interference of Two-photon Transitions (RABBITT), a phase difference between two-photon pathways involving absorption and emission of an infrared photon is extracted. Our method can be used for extraction of a phase difference between single-photon and two-photon pathways and provides a new tool for attosecond science, which is complementary to RABBITT.

physics.atom-ph↗

arXiv2016

Above-threshold ionization in neon produced by combining optical and bichromatic XUV femtosecond pulses

We consider the ionization of neon induced by a femtosecond laser pulse composed of overlapping, linearly polarized bichromatic extreme ultraviolet and infrared fields. In particular, we study the effects of the infrared light on a two-pathway ionization scheme for which Ne 2s22p53s1P is used as intermediate state. Using time-dependent calculations, supported by a theoretical approach based on the strong-field approximation, we analyze the ionization probability and the photoelectron angular distributions associated with the different sidebands of the ionization spectrum. Complex oscillations of the angular distribution anisotropy parameters as a function of the infrared light intensity are revealed. Finally, we demonstrate that coherent control of the asymmetry is achievable by tuning the infrared frequency to a nearby electronic transition.

physics.atom-ph↗

arXiv2016

Photoelectron angular distribution in two-pathway ionization of neon with femtosecond XUV pulses

We analyze the photoelectron angular distribution in two-pathway interference between non\-resonant one-photon and resonant two-photon ionization of neon. We consider a bichromatic femtosecond XUV pulse whose fundamental frequency is tuned near the $2p^5 3s$ atomic states of neon. The time-dependent Schrödinger equation is solved and the results are employed to compute the angular distribution and the associated anisotropy parameters at the main photoelectron line. We also employ a time-dependent perturbative approach, which allows obtaining information on the process for a large range of pulse parameters, including the steady-state case of continuous radiation, i.e., an infinitely long pulse. The results from the two methods are in relatively good agreement over the domain of applicability of perturbation theory.

physics.atom-ph↗

arXiv2014

Displacement effect in strong-field atomic ionization by an XUV pulse

We study strong-field atomic ionization driven by an XUV pulse with a non\-zero displacement, the quantity defined as the integral of the pulse vector potential taken over the pulse duration. We demonstrate that the use of such pulses may lead to an extreme sensitivity of the ionization process to subtle changes of the parameters of a driving XUV pulse, in particular, the ramp-on/off profile and the carrier envelope phase. We illustrate this sensitivity for atomic hydrogen and lithium driven by few-femto\-second XUV pulses with intensity in the $\rm 10^{14}~W/cm^2$ range. We argue that the observed effect is general and should modify strong-field ionization of any atom, provided the ionization rate is sufficiently high.

physics.atom-ph↗