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Physical Review Research

Influence of an atomic resonance on the coherent control of the photoionization process

Грызлова Елена Владимировна, Paolo Antonio Carpeggiani, Maria M. Popova, Maksim D. Kiselev, Nicolas Douguet, Maurizio Reduzzi, M. Negro, Antoine Comby, H. Ahmadi, V. Wanie, Mattea Carmen Castrovilli, Andreas Fischer, P. Johnsson, Michael Meyer, Klaus Bartschat, Sergei M. Burkov, Tamás Csizmadia, Mathieu Dumergue, S. Kühn, N. G. Harshitha, Miklós Füle, F. Aeenehvand, Frank Stienkemeier, Denys Iablonskyi, Kiyoshi Ueda, P. Finetti, Marco Zangrando, Nicola Mahne, Kenichi L. Ishikawa, Oksana Plekan, Kevin Charles Prince, E. Allaria, Luca Giannessi, Carlo Callegari, Alexei N. Grum-Grzhimailo, G. Sansone

Published Sep 23, 2022• 7 citations
Publisher

Abstract

In coherent control schemes, pathways connecting an initial and a final state can be independently controlled by manipulating the complex amplitudes of their transition matrix elements. For paths characterized by the absorption of multiple photons, these quantities depend on the magnitude and phase between the intermediate steps, and are expected to be strongly affected by the presence of resonances. We investigate the coherent control of the photoemission process in neon using a phase-controlled two-color extreme ultraviolet pulse with frequency in proximity of an excited energy state. Using helium as a reference, we show that the presence of such a resonance in neon modifies the amplitude and phase of the asymmetric emission of photoelectrons. Theoretical simulations based on perturbation theory are in fair agreement with the experimental observations.

DOI
10.1103/physrevresearch.4.033231

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In coherent control schemes, pathways connecting an initial and a final state can be independently controlled by manipulating the complex amplitudes of their transition matrix elements. For paths characterized by the absorption of multiple photons, these quantities depend on the magnitude and phase between the intermediate steps, and are expected to be strongly affected by the presence of resonances. We investigate the coherent control of the photoemission process in neon using a phase-controlled two-color extreme ultraviolet pulse with frequency in proximity of an excited energy state. Using helium as a reference, we show that the presence of such a resonance in neon modifies the amplitude and phase of the asymmetric emission of photoelectrons. Theoretical simulations based on perturbation theory are in fair agreement with the experimental observations.
Coherent control of interfering one- and two-photon processes has for decades been the subject of research to achieve the redirection of photocurrent. The present study develops two-pathway coherent control of ground-state helium atom above-threshold photoionization for energies up to the N=2N=2N=2 threshold, based on a multichannel quantum defect and R-matrix calculation. Three parameters are controlled in our treatment: the optical interference phase $\mathrm{\ensuremath{\Delta}}\mathrm{\ensuremath{\Phi}}$, the reduced electric field strength $\ensuremath{\chi}={\mathcal{E}}_{\ensuremath{\omega}}^{2}/{\mathcal{E}}_{2\ensuremath{\omega}}$, and the final state energy $\ensuremath{\epsilon}$. A small energy change near a resonance is shown to flip the emission direction of photoelectrons with high efficiency, through an example where 9090%90 of photoelectrons whose energy is near the 2p21Se2{p}^{2}{\phantom{\rule{4pt}{0ex}}}^{1}{S}^{e}2p21Se resonance flip their emission direction. However, the large fraction of photoelectrons ionized at the intermediate state energy, which are not influenced by the optical control, make this control scheme challenging to realize experimentally.
We present the results of our study on coherent control of photoionization of atomic barium. Our study focused on the understanding of the controllability, especially due to the effect of the coherent interaction between the atomic system and the laser field. The first half of the study investigates the mechanisms of the control behind the previously observed laser phase-insensitive product state control. The controllability of this excitation scheme, two-color two-photon resonantly enhanced excitation, was analyzed from two aspects, the role of ac Stark shift introduced by the strong laser field and the multi-pathway quantum mechanical interferences. We have analyzed the excitation scheme from the analysis of the photoelectron angular distribution measured using the excitation scheme and the monitoring of the intermediate state population. Analysis of the data as well as the numerical simulation showed clear understanding of the role of two mechanisms in the product state control reported. We also investigated the control of the phase lag during the product state control. We conducted the control of the phase lag in the study of asymmetric photoelectron angular distribution, which arises from the concurrent even-odd parity outgoing electron wave excitation. The phase lag was controlled in full range, 2π, and the results were analyzed in terms of the role of autoionizing resonance structures as well as the nature of outgoing electron waves at different locations of the autoionizing resonances.
We investigate the coherent control of the photoelectron angular distribution in bichromatic atomic ionization. Neon is selected as target since it is one of the most popular systems in current gas-phase experiments with free-electron lasers (FELSs). In particular, we tackle practical questions, such as the role of the fine-structure splitting, the pulse length, and the intensity. Time-dependent and stationary perturbation theory are employed, and we also solve the time-dependent Schr\"odinger equation in a single-active electron model. We consider neon ionized by a FEL pulse whose fundamental frequency is in resonance with either $2p\text{\ensuremath{-}}3s$ or $2p\text{\ensuremath{-}}4s$ excitation. The contribution of the nonresonant two-photon process and its potential constructive or destructive role for quantum coherent control is investigated.
We present results from perturbative calculations on a scheme of coherent control in Mg. The scheme involves the excitation of Mg in the vicinity of an autoionizing resonance lying above the first two ionization thresholds by a two-color field composed of a fundamental frequency and its third harmonic, whose relative phase can be continuously controlled. Four as well as two-photon coherent excitation pathways, involving appropriate combinations of the two frequencies, proceed through the atomic continuum simultaneously contributing to the excitation, while three-photon ionization by the fundamental is also energetically possible. As a result, some of the excitation processes involve above-threshold ionization (ATI). The calculated ionization yields for the various groups of photoelectrons reveal significant modulation as the relative phase of the field component frequencies is varied. The modulation patterns for the different photoelectron groups are mutually shifted due to the multiphoton matrix element phases associated both with the ATI process and the multichannel nature of the final state. The effect is particularly pronounced when the autoionizing state is in near four-photon resonance with the fundamental frequency. The role of an autoionizing state as a final state as well as that of the continuum as an intermediate state in coherent control processes is discussed.
Abstract We present a theoretical study on the quantum control of ultrafast Rabi dynamics in atoms driven by chirped extreme ultraviolet (XUV) pulses. Motivated by recent experimental advances using free-electron lasers, we derive an analytical solution of the Rabi oscillation under the rotating wave approximation, incorporating the spectral chirp of the XUV field. Within the essential-states model, we demonstrate how the chirp modulates the phase of the excited-state amplitude, inducing an observable asymmetry in the Autler–Townes (AT) doublets of the photoelectrons. Our theoretical predictions, benchmarked against time-dependent Schrödinger equation simulations, reveal that chirp-dependent phase modulation governs the spectral asymmetry, offering a time-domain perspective for interpreting strong-field photoionization at short wavelengths. This work provides a compact analytical framework for chirp-mediated coherent control in the XUV regime and sheds light on recent experimental observations of asymmetric AT structures in helium.
Abstract Coherent control uses interference between quantum pathways to enhance or suppress transitions to a target quantum state. In stimulated Raman excitation, such control can be achieved through interference between two indistinguishable pathways connecting the same initial and final states, with the relative phase between the pathways modulating the population transfer to the final state. Extending this strategy to the extreme ultraviolet (XUV) and X-ray regimes would enable control of ultrafast electronic dynamics and site-selective core excitations. However, Raman coupling at short wavelengths competes with photoionization and intermediate-state decay, whereas intense fields with stable and adjustable relative phases remain difficult to produce. Here we use two-colour pulses from a seeded coherent free-electron laser to excite helium from its ground state to a bound metastable state via stimulated XUV Raman excitation. We implement phase-coherent control by creating two interfering Raman pathways through the ionization continuum and modulate the transferred population by varying their relative phases. Blocking one pathway removes the modulation, confirming its interferometric origin, and time-dependent Schrödinger equation calculations reproduce the measured phase dependence. Our results establish phase-controlled stimulated Raman excitation in the XUV regime, providing a strategy for the coherent control of atomic and molecular processes at short wavelengths.