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Vladislav V. Serov

Publications and source records attributed to Vladislav V. Serov.

At least 19 recordsLinked to original sources

Rainbow RABBITT as a Probe of Coherent Rabi Dynamics

Attosecond pulse trains interacting with a resonantly dressed atom generate a pronounced intra-sideband phase structure that remains hidden in conventional spectrally integrated RABBITT measurements. Using \textit{ab initio} time-dependent Schrödinger equation calculations for lithium near the resonant $2s\to2p$ transition, we show that the phase extracted within a single sideband can vary by nearly $π$ across its spectral width. The resulting intra-sideband phase dispersion exhibits a characteristic dependence on the IR detuning, pulse duration, intensity, and sideband order. Most strikingly, exact resonant Rabi flopping flattens the intra-sideband phase dispersion, whereas a small detuning generates a pronounced phase modulation despite weaker population transfer. This counterintuitive behavior demonstrates that rainbow RABBITT probes the dynamical phase accumulated by a Rabi-dressed wave packet rather than the instantaneous populations of the participating states. A simple analytical model captures the principal features of the numerical calculations and provides physical insight into the emergence of the intra-sideband phase structure. These results establish intra-sideband phase dispersion as a new interferometric observable for mapping coherent Rabi dynamics.

physics.atm-clus↗

Circular RABBITT goes under threshold

We introduce circular under-threshold RABBITT (cuRABBITT) as a new interferometric method to probe discrete electronic excitations in atoms with attosecond resolution. By combining circularly polarized attosecond pulses with broadband (``rainbow'') spectral analysis, we directly access two-photon ionization amplitudes and their relative phases. Time-dependent Schrödinger simulations, supported by Green's function theory, reveal strong resonances in helium and argon and a Cooper-like minimum in xenon. These results demonstrate that cuRABBITT provides continuous spectral mapping of bound-state resonances and extends Fano's propensity rule into the under-threshold regime. Our work establishes cuRABBITT as a powerful attosecond metrology technique, opening the way to polarization-resolved studies of resonant dynamics in atoms and molecules.

physics.atom-ph↗

Fano line shape metamorphosis in resonant two-photon ionization

Two-photon atomic ionization driven by time-locked XUV and IR pulses allows to study dynamics of Fano resonances in time and energy domains. Different time evolution of the two interfering pathways leading to a Fano resonance can be exploited to turn the Fano profile of the two-photon XUV/IR ionization into a symmetric Gaussian once the directly ejected photoelectron leaves the parent ion and cannot any longer absorb an IR photon. This line shape transformation allows for the direct determination of the resonant lifetime from the spectroscopic measurements without need for an extremely fine energy resolution. Ubiquitous nature of Fano resonances makes this determination a universal tool in diverse quantum systems ranging from nuclei to nano-fabricated solids.

physics.atom-ph↗

Time-dependent convergent close coupling method for molecular ionization in laser fields

We develop a time-dependent multi-configurational numerical technique for calculating ionization by short laser pulses of many-electron molecules. The method is based on the expansion of the wave function of a molecule into the eigenstates of the molecular ion. We classify this method as time-dependent convergent close coupling (TDCCC) because it uses the same symmetry for channel functions as the well-known convergent close coupling (CCC) method.

physics.atom-ph↗

XUV ionization of the H$_2$ molecule studied with attosecond angular streaking

We study orientation and two-center interference effects in attosecond time-resolved photoionization of the H$_2$ molecule. Time resolution of XUV ionization of H$_2$ is gained through the phase retrieval capability of attosecond angular streaking demonstrated earlier by Kheifets {\em et al} [arXiv:2202.06147 (2022)]. Once applied to H$_2$, this technique delivers an anisotropic phase and time delay which both depend sensitively on the molecular axis orientation. In addition, the photoelectron momentum distribution displays a very clear two-center interference pattern. When the interference formula due to Walter and Briggs [J. Phys. B {\bf 32} 2487 (1999)] is applied, an effective photoelectron momentum appears to be greater than the asymptotic momentum at the detector. This effect is explained by a molecular potential well surrounding the photoemission center.

physics.atom-ph↗

Numerical attoclock on atomic and molecular hydrogen

Numerical attoclock is a theoretical model of attosecond angular streaking driven by a very short, nearly a single oscillation, circularly polarized laser pulse. The reading of such an attoclock is readily obtained from a numerical solution of the time-dependent Schrödinger equation as well as a semi-classical trajectory simulation. By making comparison of the two approaches, we highlight the essential physics behind the attoclock measurements. In addition, we analyze the predictions of the Keldysh-Rutherford model of the attoclock [Phys. Rev. Lett. 121, 123201 (2018)]. In molecular hydrogen, we highlight a strong dependence of the width of the attoclock angular peak on the molecular orientation and attribute it to the two-center electron interference. This effect is further exemplified in the weakly bound neon dimer.

physics.atom-ph↗

Time delay in XUV/IR photoionization of H$_2$O

We solve the time-dependent Schrödinger equation describing a water molecule driven by a superposition of the XUV and IR pulses typical for a RABBITT experiment. This solution is obtained by a combination of the time-dependent coordinate scaling and the density functional theory with self-interaction correction. Results of this solution are used to determine the time delay in photoionization of the water and hydrogen molecules.

physics.atom-ph↗

Orthogonal fast spherical Bessel transform on uniform grid

We propose an algorithm for the orthogonal fast discrete spherical Bessel transform on an uniform grid. Our approach is based upon the spherical Bessel transform factorization into the two subsequent orthogonal transforms, namely the fast Fourier transform and the orthogonal transform founded on the derivatives of the discrete Legendre orthogonal polynomials. The method utility is illustrated by its implementation for the numerical solution of the three-dimensional time-dependent Schrödinger equation.

math.NA↗

Angular anisotropy of time delay in XUV/IR photoionization of H$_2^+$

We develop a novel technique for modeling of atomic and molecular ionization in superposition of XUV and IR fields with characteristics typical for attosecond streaking and RABBITT experiments. The method is based on solving the time-dependent Schrödinger equation in the coordinate frame expanding along with the photoelectron wave packet. The efficiency of the method is demonstrated by calculating angular anisotropy of photoemission time delay of the H$_2^+$ ion in a field configuration of recent RABBITT experiments.

physics.atom-ph↗

Solution of the Schrödinger equation using exterior complex scaling and fast Fourier transform

The split-operator pseudo-spectral method based on the fast Fourier transform (SO-FFT) is a fast and accurate method for the numerical solution of the time-dependent Schrödinger-like equations (TDSE). As well as other grid-based approaches, SO-FFT encounters a problem of the unphysical reflection of the wave function from the grid boundaries. Exterior complex scaling (ECS) is an effective method widely applied for the suppression of the unphysical reflection. However, SO-FFT and ECS have not been used together heretofore because of the kinetic energy operator coordinate dependence that appears in ECS applying. We propose an approach for the combining the ECS with SO-FFT for the purpose of the solution of TDSE with outgoing-wave boundary conditions. Also, we propose an effective ECS-friendly FFT-based preconditioner for the solution of the stationary Schrödinger equation by means of the preconditioned conjugate gradients method.

physics.atom-ph↗

Time-dependent calculations of transfer ionization by fast proton-helium collision in one-dimensional kinematics

We analyze a transfer ionization (TI) reaction in the fast proton-helium collision $\rm H^+ + He \to H^0 + He^{2+} + e^-$ by solving a time-dependent Schrödinger equation (TDSE) under the classical projectile motion approximation in one-dimensional kinematics. In addition, we construct various time independent analogues of our model using lowest order perturbation theory in the form of the Born series. By comparing various aspects of the TDSE and the Born series calculations, we conclude that the recent discrepancies of experimental and theoretical data may be attributed to deficiency of the Born models used by other authors. We demonstrate that the correct Born series for TI should include the momentum space overlap between the double ionization amplitude and the wave function of the transferred electron.

physics.atom-ph↗

The p-H symmetry breaking in dissociative ionization of H2 due to the molecular ion interaction with the ejected electron

We propose a novel mechanism of electron localization and molecular symmetry breaking in dissociative photoionization of the H$_2$ molecule. The Coulomb field of the ejected electron can induce transition of the remaining H$_2^+$ ion from the gerade $^2Σ_g^1(1sσ_g)$ to the ungerade $^2Σ_u^1(2pσ_u)$ electronic state when the nuclei in a bound vibrational state are near the outer turning point. The superposition of this process with a direct transition to vibrational continuum should produce a non-gerade ionic state which results in observed asymmetry in the $p$-H ejection relative to the electron ejection direction at a small kinetic energy release.

physics.atom-ph↗

Intermediate-energy electron-impact dissociative ionization-excitation of molecular hydrogen

We have implemented three variants of the exterior complex scaling procedure in prolate spheroidal coordinates (PS-ECS) to study the dissociative electron impact ionization-excitation of hydrogen molecule, where the emerging electrons and one of the protons are detected in coincidence for the first time in a recent experiment. In the first variant, designated PSECS-1B, the two target electrons are treated ab initio while the interaction of the incident-scattered electron is taken into account using the first term of the Born series. In the second, PSECS-2BCD, the second Born term is introduced in the dipole approximation. In the third approach, designated PSECS-SW, applied to the ionization-excitation to the $2pσ_u$ level of H$_2^+$, the multi-configurational single active electron approximation is used for the target, while the interaction of the incident electron with the target is described ab initio. Our results agree partially with those of a recent experiment which is in progress.

physics.atom-ph↗

The hybrid surface flux method for the ionization amplitude extraction from the calculated wavefunction

A method is proposed for extracting ionization amplitudes from the solution of the time-dependent Schrödinger equation (TDSE) describing a system in a time-dependent external field. The method is a hybrid of two earlier developed methods, the time-dependent surface flux (t-SURFF) method and the method using the propagated wavepacket as the source term in a time-independent driven Schrödinger equation with the field-free Hamiltonian. It is demonstrated that the method combines the advantages of the parent ones and allows the extraction of ionization amplitudes by solving the TDSE within a small spatial domain (with the boundary conditions provided by exterior complex scaling) and a time interval, not exceeding the external field pulse duration.

physics.atom-ph↗

Interpretation of the time delay in the ionization of Coulomb and two-center systems

We consider the time delay of electron detachment from a Coulomb center and two-center systems in the process of ionization. It is shown that the attosecond streaking, most usual method of time delay measure, can be formally described by placing a virtual detector of the arrival time delay at a certain distance from the center of the system. This approach allows derivation of a simple formula for Coulomb-laser coupling that perfectly agrees with the results of numerical solution of the time-dependent Schrodinger equation. The dependence of the time delay upon the energy, the angular momentum projection, and the azimuthal quantum number is studied for the ionization of molecular hydrogen ion. Finally, we propose a physical interpretation of singularities, arising when the formal expression for the time delay is applied to the ionization of molecular hydrogen.

physics.atom-ph↗

Calculation of intermediate-energy electron-impact ionization of molecular hydrogen and nitrogen using the paraxial approximation

We have implemented the paraxial approximation followed by the time-dependent Hartree-Fock method with frozen core for the single impact ionization of atoms and two-atomic molecules. It reduces the original scattering problem to the five-dimensional time-dependent Schrödinger equation solution. By using this method we calculated the multi-fold differential cross section of the impact single ionization of the helium atom, the hydrogen molecule and the nitrogen molecule by the intermediate energy electrons. Our results for the helium and the hydrogen are quite close to experimental data, but for N$_2$ the agreement is worse apparently because of the insufficiency of the frozen core approximation.

physics.atom-ph↗

Modern methods for calculations of photoionization and electron impact ionization of two-electron atoms and molecules

A review of some recently developed methods of calculating multiple differential cross-sections of photoionization and electron impactionization of atoms and molecules having two active electrons is presented. The methods imply original approaches to calculating three-particle Coulomb wave functions. The external complex scaling method and the formalism of the Schroedinger equation with a source in the right-hand side are considered. Efficiency of the time-dependent approaches to the scattering problem, such as the paraxial approximation and the time-dependent scaling, is demonstrated. An original numerical method elaborated by the authors for solving the 6D Schroedinger equation for an atom with two active electrons, based on the Chang-Fano transformation and the discrete variable representation, is formulated. Basing on numerical simulations, the threshold behavior of angular distributions of two-electron photoionization of the negative hydrogen ion and helium atom, and multiple differential cross-sections of electron impact ionization of hydrogen and nitrogen molecules are analyzed. It is demonstrated that the Wannier law for the angular distribution of double ionisation is not correct even at very small energies.

physics.atom-ph↗

Is the Wannier threshold law for angular distribution in double photoionization of atoms true at practically attainable energies of ejected electrons?

We calculated ab initio the three-fold differential cross section of a double single-photon Helium photoionization at equal energy sharing, and obtained from one the Gaussian width parameter, describing the angular interelectron correlations, for the total electrons energies range E from 0.1 eV to 100 eV. The results are in excellent agreement with experimental data but indicate that the Wannier threshold law for angular distribition is not correct at energies attainable in modern experiments. It is shown that the Gaussian width parameter dependence on energy is much better described by the modified threshold law, obtained by Kazansky and Ostrovsky [J. Phys. B 26, 2231 (1993)]. Also, we explored the Gaussian width parameter for a double photoionization of the targets with the strongly asymmetrical initial state configuration: the atomic Hydrogen negative ion and the Helium in the 2s1S and 3s1S excited states. We found that the Gaussian width parameter dependence on the total ejected electrons energy for this targets has a maximum at low energies. We show also that the correlation parameter dependence on the interelectron angle for these targets is essentially non-Gaussian and has a number of peaks equal to a number of initial state radial nodes, that reveals the new abilities for the qualitative analysis of electron structure.

physics.atom-ph↗