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Physical Review A

Interfering one-photon and two-photon ionization by femtosecond VUV pulses in the region of an intermediate resonance

Alexei N. Grum-Grzhimailo, Грызлова Елена Владимировна, Ekaterina I. Staroselskaya, Joel Venzke, Klaus Bartschat

Published Jun 25, 2015• 38 citations
Publisher

Abstract

The electron angular distribution after atomic photoionization by the fundamental frequency and its second harmonic is analyzed for a case when the frequency of the fundamental scans the region of an intermediate atomic state. The angular distribution and its left-right asymmetry, due to the two-pathway interference between nonresonant one-photon and resonant two-photon ionization, sharply change as a function of the photon energy. The phenomenon is exemplified by both solving the time-dependent Schr\"odinger equation on a numerical space-time grid and by applying perturbation theory for ionization of the hydrogen atom in the region of the $1s\text{\ensuremath{-}}2p$ transition for femtosecond pulses as well as an infinitely long exposure to the radiation. Parametrizations for the asymmetry and the anisotropy coefficients, obtained within perturbation theory, reveal general characteristics of observable quantities as functions of the parameters of the radiation beam.

DOI
10.1103/physreva.91.063418

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arXiv:1110.1139•Physical Review Letters•Jan 19, 2012•78 citations
The electron angular distribution after atomic photoionization by the fundamental frequency and its second harmonic is analyzed for a case when the frequency of the fundamental scans the region of an intermediate atomic state. The angular distribution and its left-right asymmetry, due to the two-pathway interference between nonresonant one-photon and resonant two-photon ionization, sharply change as a function of the photon energy. The phenomenon is exemplified by both solving the time-dependent Schr"odinger equation on a numerical space-time grid and by applying perturbation theory for ionization of the hydrogen atom in the region of the 1s\ensuremath-2p1s\text{\ensuremath{-}}2p1s\ensuremath-2p transition for femtosecond pulses as well as an infinitely long exposure to the radiation. Parametrizations for the asymmetry and the anisotropy coefficients, obtained within perturbation theory, reveal general characteristics of observable quantities as functions of the parameters of the radiation beam.
We investigate two-pathway interferences between nonresonant one-photon and resonant two-photon ionization of atomic hydrogen. In particular, we analyze in detail the photoionization mediated by the fundamental frequency and the second harmonic of a femtosecond VUV pulse when the fundamental is tuned near an intermediate atomic state. Following our recent study [Phys. Rev. A 91, 063418 (2015)] of such effects with linearly polarized light, we analyze a similar situation with circularly polarized radiation. As a consequence of the richer structure in circularly polarized light, characterized by its right-handed or left-handed helicity, we present and discuss various important features associated with the photoelectron angular distribution.
We theoretically study the photoelectron angular distribution (PAD) from the two-photon single ionization of H and He by femtosecond and attosecond extreme-ultraviolet pulses, based on the time-dependent perturbation theory and simulations with the full time-dependent Schrodinger equation. The PAD is formed by the interference of the s and d continuum wave packets, and, thus, contains the information on the relative phase and amplitude ratio between them. We find that, when a spectrally broadened femtosecond pulse is resonant with an excited level, the PAD substantially changes with pulse width, since the competition between resonant and nonresonant ionization paths, leading to distinct from the scattering phase shift difference, changes with it. In contrast, when the Rydberg manifold is excited, and for the case of above-threshold two-photon ionization, and the PAD do not depend much on pulse width, except for the attosecond region. Thus, the Rydberg manifold and the continuum behave similarly in this respect. For a high-harmonic pulse composed of multiple harmonic orders, while the value is different from that for a single-component pulse, the PAD still rapidly varies with pulse width. The present results illustrate a new way to tailor the continuum wave packet.
By numerically solving the three-dimensional time-dependent Schr\"odinger equation, two-photon ionization of hydrogen is investigated at the near-resonant frequencies of the $1s\text{\ensuremath{-}}2p$ transition. Due to the Rabi oscillations between the 1s1s1s and 2p2p2p states, the photoelectron energy spectra exhibit the Autler-Townes (AT) doublets and we focus on the energy spacing and the asymmetry of the doublets. Our results show that the laser frequency for the minimum energy spacing of AT doublets locates at the resonant frequency of the ac-stark-shifted states, while the symmetry of the AT doublets is affected both by the ac-stark shift and the nonresonant ionization pathway. Developing the minimal three-state model including all of the nonresonant (nonessential) states, the effects of the ac-stark shift and the nonresonant ionization pathway on the AT doublets due to the nonresonant states are identified. Furthermore, due to the nonresonant ionization pathway, the photoelectron angular distributions are distinctly different for the lower- and higher-energy peaks in the AT doublets and these angular distributions sensitively depend on the laser intensity and pulse duration. These results are well reproduced by our minimal three-state model.
We present a theoretical study of the main characteristics of two-color photoionization spectra obtained when atoms are subjected to an intense radiation pulse containing the fundamental of an infrared laser and one of its higher harmonics. The frequency of the latter is chosen to be high enough that the atom can be ionized by a single photon. The calculation is performed by numerical integration of the time-dependent Schrödinger equation for a (three-dimensional) hydrogen atom. We present the general properties of the spectra and angular distributions as well as the possible occurrence of interferences between the laser-assisted process and above-threshold ionization. Our results indicate that such interference effects, which can lead to partial coherent control of the photoionization process, can be observed at moderate laser intensities within the reach of currently operated laser and harmonic sources.
We theoretically study the pulse-width dependence of the photoelectron angular distribution (PAD) from the resonance-enhanced two-photon single ionization of He by femtosecond (≲20 fs) extreme-ultraviolet pulses, based on the time-dependent perturbation theory and simulations with the full time-dependent Schrödinger equation. In particular, we focus on the competition between resonant and nonresonant ionization paths, which leads to the relative phase δ between the S and D wave packets distinct from the corresponding scattering phase shift difference. When the spectrally broadened pulse is resonant with an excited level, the competition varies with pulse width, and, therefore, δ and the PAD also change with it. On the other hand, when the Rydberg manifold is excited, δ and the PAD do not much vary with the pulse width, except for the very short-pulse regime.