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Anatoli S. Kheifets

Publications and source records attributed to Anatoli S. Kheifets.

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↗

Attosecond Time Delays at Cooper Minima in Valence-Shell Photoionization of Alkali and Alkaline-Earth Metal Atoms

Ji \etal [New J. Phys. {\bf 26}, 093014 (2024)] established a direct link between the photoionization cross section and the attosecond time delay near Cooper minima (CM) in the valence shells of noble-gas atoms. This link is based on the analytic properties of the ionization amplitude in the complex plane of the photoelectron energy, and is particularly sensitive to the winding number of the amplitude around the origin of the complex energy plane. % Here, we demonstrate an analogous relation for photoionization of the valence $ns$ shells of alkali-metal atoms (AMA), from Na ($n=3$) to Cs ($n=6$), as well as alkaline-earth-metal atoms (AEMA), from Mg ($n=3$) to Ba ($n=6$). To this end, we employ a fully relativistic formalism that separates the two complementary $ns_{1/2} \to Ep_{1/2}$ and $Ep_{3/2}$ ionization channels. Each of these channels exhibits a phase variation close to $π$, but in opposite directions, near their respective Cooper minima. This phase variation vanishes in a nonrelativistic formulation, where the two channels become degenerate % For AMA, due to the threshold proximity of the CM, the universal Coulomb contribution to the time delay must be subtracted. The remaining component of the time delay is target-specific, angular-dependent, and accessible through comparative measurements.

physics.atom-ph↗

Resonant photoionization and time delay

Resonances leave prominent signatures in atomic and molecular ionization triggered by the absorption of single or multiple photons. These signatures reveal various aspects of the ionization process, characterizing both the initial and final states of the target. Resonant spectral features are typically associated with sharp variations in the photoionization phase, providing an opportunity for laser-assisted interferometric techniques to measure this phase and convert it into a photoemission time delay. This time delay offers a precise characterization of the timing of the photoemission process. In this review, a unified approach to resonant photoionization is presented by examining the analytic properties of ionization amplitude in the complex photoelectron energy plane. This approach establishes a connection between the resonant photoemission time delay and the corresponding photoionization cross-section. Numerical illustrations of this method include: (i) giant or shape resonances, where the photoelectron is spatially confined within a potential barrier, (ii) Fano resonances, where bound states are embedded in the continuum, (iii) Cooper minima (anti-resonances) arising from kinematic nodes in the dipole transition matrix elements, and (iv) confinement resonances in atoms encapsulated within a fullerene cage. The second part of this review focuses on two-photon resonant ionization processes, where the photon energies can be tuned to a resonance in either the intermediate or final state of the atomic target. Our examples include one- or two-electron discrete excitations both below and above the ionization threshold. These resonant states are probed using laser-assisted interferometric techniques. Additionally, we employ laser-assisted photoemission to measure the lifetimes of several atomic autoionizing states.

physics.atom-ph↗

Relation Between Photoionisation Cross Sections and Attosecond Time Delays

Determination and interpretation of Wigner-like photoionisation delays is one of the most active fields of attosecond science. Previous results have suggested that large photoionisation delays are associated with structured continua, but a quantitative relation between photoionisation cross sections and time delays has been missing. Here, we derive a Kramers-Kronig-like relation between these quantities and demonstrate its validity for (anti)resonances. This new concept defines a topological analysis, which rationalises the sign of photoionisation delays and thereby sheds new light on a long-standing controversy regarding the sign of the photoionisation delay near the Ar 3s Cooper minimum. Our work bridges traditional photoionisation spectroscopy with attosecond chronoscopy and offers new methods for analysing and interpreting photoionisation delays.

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↗

Polarization control of RABBITT in noble gas atoms

The mutual angle formed by the non-collinear polarization axes of two laser pulses is used to control two-photon XUV+IR ionization of noble gas atoms in the process of reconstruction of attosecond bursts by beating of two-photon transitions (RABBITT). The magnitude and the phase of this beating can be controlled very efficiently by the mutual polarization angle. The mechanism of this control can be understood within the lowest order perturbation theory and the soft photon approximation. We offer a very sensitive test on the polarization control of the angular dependent RABBITT process which validates our numerical simulations. We apply this test to the recent theoretical and experimental results of polarization controlled RABBITT on hydrogen and helium by Boll et al., Phys. Rev. A 107, 043113 (2023) and heavier noble gases by Jiang et~al., Nature Comms. 13, 5072 (2022).

physics.atom-ph↗

Shape resonances in photoionization cross sections and time delay

Shape resonances in photoionization of atoms and molecules arise from a particular geometry of the ionic potential which traps the receding photoelectron in a quasi-bound state in a particular partial wave. This mechanism allows us to connect the photoionization cross section in the resonant region with the photoelectron scattering phase in this partial wave by a simple formula $σ\propto \sin^2δ_\ell$. Due to this relation, the phase $δ_\ell$ can be extracted from an experimentally known cross section and then converted to the photoelectron group delay (Wigner time delay) $τ_{\rm W} = \partial δ_\ell/\partial E$ which is measurable by recently developed laser interferometric techniques. Such a direct connection of the photoionization cross section and the time delay is a fundamental property of shape resonances which provides a comprehensive test of novel measurements against a large body of older synchrotron data.

physics.atom-ph↗

Phase retrieval from angular streaking of XUV atomic ionization

We demonstrate an accurate phase retrieval of XUV atomic ionization by streaking the photoelectron in a circularly polarized IR laser field. The streaking phase can then be converted to the atomic time delay containing the Wigner and continuum-continuum components. Our demonstration is based on a numerical solution of the time-dependent Schrödinger equation. We test this technique using the hydrogen atom ionized by an isolated attosecond XUV pulse across a wide range of photon energies. In parallel, we run a series of RABBITT simulations and demonstrate equivalence of the phase and timing information provided by the two methods. This validates the proposed technique and makes it a useful tool that can be applied to a broad range of atomic and molecular targets exposed to XUV radiation from novel free-electron laser sources.

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↗

Strongly resonant RABBITT on lithium

The process of reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) can become resonant with a discrete atomic level either in the intermediate or the final continuous states. Experimental observations of the former [Phys. Rev. Lett. 104, 103003 (2010)] or latter [Nat. Commun. 7, 10566 (2016)] cases revealed modification of only those parts of the photoelectron spectrum that overlapped directly with the resonance. In the lithium atom and other members of the alkali metal family, the valence shell $ns\to np$ transition to the intermediate RABBITT state affects the whole photoelectron spectrum in the final state. The strong additional resonant channel modifies entirely the ionization dynamics and opens direct access to the resonant phase of the two-photon transitions which is common for various single and multiple electron ionization processes. Elucidation of this phase has wider implications for strongly resonant laser-matter interaction.

physics.atom-ph↗

Effect of the finite speed of light in ionization of extended systems

We study propagation effects due to the finite speed of light in ionization of extended systems. We present a general quantitative theory of these effects and show under which conditions such effects should appear. The finite speed of light propagation effects are encoded in the non-dipole terms of the time-dependent Shrödinger equation and display themselves in the photoelectron momentum distribution projected on the molecular axis. Our numerical modeling for the \Hp molecular ion and the \Ne dimer shows that the finite light propagation time from one atomic center to another can be accurately determined in a table top laser experiment which is much more readily affordable than an earlier synchrotron measurement by Grundmann {\em et al} [Science 370, 339 (2020)]

physics.atom-ph↗

The attoclock and the tunnelling time debate

Attosecond angular streaking, also known as the "attoclock", employs a short elliptically polarized laser pulse to tunnel ionize an electron from an atom or a molecule and to put a time stamp on this process by deflecting the photoelectron in the angular spatial direction. This deflection can be used to evaluate the time the tunneling electron spends under the classically inaccessible barrier and to determine whether this time is finite. In this review, we examine the latest experimental and theoretical findings and present a comprehensive set of evidence supporting the zero tunneling time scenario.

physics.atom-ph↗

Correlation enhancement of high-order harmonics generation in Xe

We consider the process of high-order harmonics generation (HHG) in the xenon atom enhanced by the inter-shell correlation between the valence 5p and inner 4d shells. We derive the HHG spectrum from a numerical solution of the one-electron time-dependent Schrödinger equation multiplied by the enhancement factor taken as the photoionization cross-sections ratio calculated with and without the inter-shell correlation. Such a simplified approach is adequate to describe the experimental HHG spectrum reported by Shiner et al [Nat. Phys. 7, 464 (2011)] generated by a single color IR laser. Similarly, we find good agreement when applied to the two-color driven HHG spectra reported by Facciala et al [Phys. Rev. Lett. 117, 093902 (2016)].

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↗

Simulation of angular resolved RABBITT measurements in noble gas atoms

We simulate angular resolved RABBITT (Reconstruction of Attosecond Beating By Interference of Two-photon Transitions) measurements on valence shells of noble gas atoms (Ne, Ar, Kr, and Xe). Our non-perturbative numerical simulation is based on solution of the time-dependent Schrödinger equation for a target atom driven by an ionizing XUV and dressing IR fields. From these simulations we extract the angular dependent magnitude and phase of the RABBITT oscillations and deduce the corresponding angular anisotropy β parameter and Wigner time delay $τ_W$ for the single XUV photon absorption which initiates the RABBITT process. Said β and $τ_W$ parameters are compared with calculations in the random phase approximation with exchange (RPAE) which includes inter-shell correlation. This comparison is used to test various effective potentials employed in the one-electron TDSE. In lighter atoms (Ne and Ar), several effective potentials are found to provide accurate simulation of RABBITT measurements for a wide range of photon energies up to 100 eV above the valence shell threshold. In heavier atoms (Kr and Xe), the onset of strong correlation with the d-shell restricts the validity of the single active electron approximation to several tens of eV above the valence shell threshold.

physics.atom-ph↗

Keldysh-Rutherford model for attoclock

We demonstrate a clear similarity between attoclock offset angles and Rutherford scattering angles taking the Keldysh tunnelling width as the impact parameter and the vector potential of the driving pulse as the asymptotic velocity. This simple model is tested against the solution of the time-dependent Schrödinger equation using hydrogenic and screened (Yukawa) potentials of equal binding energy. We observe a smooth transition from a hydrogenic to 'hard-zero' intensity dependence of the offset angle with variation of the Yukawa screening parameter. Additionally we make comparison with the attoclock offset angles for various noble gases obtained with the classical-trajectory Monte Carlo method. In all cases we find a close correspondence between the model predictions and numerical calculations. This suggests a largely Coulombic origin of the attoclock offset angle and casts further doubt on its interpretation in terms of a finite tunnelling time.

physics.atom-ph↗

Time delay anisotropy in photoelectron emission from the isotropic ground state of helium

Time delays of electrons emitted from an isotropic initial state and leaving behind an isotropic ion are assumed to be angle-independent. Using an interferometric method involving XUV attosecond pulse trains and an IR probe field in combination with a detection scheme, which allows for full 3D momentum resolution, we show that measured time delays between electrons liberated from the $1s^2$ spherically symmetric ground state of helium depend on the emission direction of the electrons relative to the linear polarization axis of the ionizing XUV light. Such time-delay anisotropy, for which we measure values as large as 60 attoseconds, is caused by the interplay between final quantum states with different symmetry and arises naturally whenever the photoionization process involves the exchange of more than one photon in the field of the parent-ion. With the support of accurate theoretical models, the angular dependence of the time delay is attributed to small phase differences that are induced in the laser-driven continuum transitions to the final states. Since most measurement techniques tracing attosecond electron dynamics involve the exchange of at least two photons, this is a general, significant, and initially unexpected effect that must be taken into account in all such photoionization measurements.

physics.atom-ph↗