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Physical Review A

Above-threshold ionization of atoms irradiated by sinusoidally phase-modulated pulses

Haiying Yuan, Yujun Yang, Fu-Ming Guo, Ji-Gen Chen, Jun Wang, Zhiwen Cui

Published Feb 5, 2024• 5 citations
Publisher

Abstract

By solving the time-dependent Schr\"odinger equation in momentum space, the photoelectron emission from atoms under the irradiation of 400 nm sinusoidal phase-modulated shaped pulses was investigated. It was found that by controlling the phase and amplitude of the pulses in the frequency domain, in addition to the photoelectron peaks generated by the interference of multiple-cycle ionization, additional resonant peak structures and interference phenomena can be observed in the photoelectron emission spectrum. Through the analysis of photoelectrons from different subpulses within the shaped pulse, it was discovered that these structures arise from the modulation of ionization and excitation processes by multiple subpulses within the shaped pulse. This study demonstrates the significant importance of utilizing shaped pulses for the control of photoelectron emission.

DOI
10.1103/physreva.109.023104

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By solving the time-dependent Schr"odinger equation in momentum space, the photoelectron emission from atoms under the irradiation of 400 nm sinusoidal phase-modulated shaped pulses was investigated. It was found that by controlling the phase and amplitude of the pulses in the frequency domain, in addition to the photoelectron peaks generated by the interference of multiple-cycle ionization, additional resonant peak structures and interference phenomena can be observed in the photoelectron emission spectrum. Through the analysis of photoelectrons from different subpulses within the shaped pulse, it was discovered that these structures arise from the modulation of ionization and excitation processes by multiple subpulses within the shaped pulse. This study demonstrates the significant importance of utilizing shaped pulses for the control of photoelectron emission.
We theoretically investigate the photoelectron emission from an atom irradiated by an amplitude modulated sinusoidally phase-modulated pulse through solving the time-dependent Schrödinger equation in the momentum space. By controlling the phase amplitude of the pulse in the frequency domain, it can be found that the photoelectron spectra appear as explicit interference phenomena, which originated from the interference between the directly ionized electron and the ionization of the pre-excited atom from different subpulses.
The dynamics of the bound-state populations and the photoelectron spectra are calculated for model atomic systems irradiated by a pulse with a harmonically modulated frequency. For a system including a single bound state a model is adopted, which takes into account the threshold behavior typical of negative ions and admits continuum-continuum transitions. For a model one-dimensional atom the results are obtained through a numerical integration of the Schr\"odinger equation. The case of a resonant ionization is also considered. The modulation of the frequency results in changing the instantaneous rate of decay of the initial state, in inducing additional population oscillations for multilevel systems, and in additional peaks in the photoelectron spectra.
We theoretically investigate the resonant two-photon ionization of a hydrogen atom in the counter-rotating circularly polarized double-pulse sequences, by solving the time-dependent Schr\"odinger equation. Due to the induced Rabi oscillations between the ground and excited states, the well-known Autler-Townes doublet is observed in the photoelectron spectra. More interestingly, our numerical results reveal an additional peak located between the Autler-Townes doublets, which originates from single-photon ionization from the excited state by the second pulse. By adjusting the laser intensity of the two pulses, the photoelectron yields of the three peaks can be sensitively modulated, under the control of completed Rabi cycles within the first pulse. In addition, our results show a potential of manipulating the photoemission anisotropy by both the laser intensity and the two-pulse time delay, through adjusting the competition of different partial waves generated by the two pulses.
We study the Rabi flopping of the population between the ground and excited 2p states of the hydrogen atom, induced by intense short laser pulses of different shapes and of carrier frequency ω=0.375 a.u. which resonantly couples the two states, and manifestations of this dynamics in the energy spectra of photoelectrons produced in the subsequent ionization of the atom from the excited state. It is found that, for Gaussian, half-Gaussian and rectangular pulses, characterized by the same pulse area, the final populations take the same values and the spectra consist of similar patterns having the same number of peaks and approximately the same separation between the prominent edge (Autler–Townes) peaks. The additional analysis in terms of dressed states showed that the mechanism of formation of multiple-peak structures during the photoionization process is the same regardless of the pulse shape. These facts disprove the hypothesis proposed in earlier studies with Gaussian pulse, that the multiple-peak pattern appears due to dynamic interference of the photoelectrons emitted with a time delay at the rising and falling sides of the pulse, since the hypothesis is not applicable to either a half-Gaussian pulse that has no rising part or a rectangular pulse whose intensity is constant.
We propose a scheme to control the shape of the Autler-Townes (AT) doublet in the photoelectron spectrum from atomic resonance-enhanced multiphoton ionization (REMPI). The scheme is based on the interference of two AT doublets created by ionization of the strongly driven atom from the ground and the resonantly excited state using tailored bichromatic femtosecond laser pulses. In this scheme, the quantum phase of the photoelectrons is crucial for the manipulation of the AT doublet. The laser polarization state and the relative optical phase between the two colors are used to manipulate the interference pattern. We develop an analytical model to describe the bichromatic REMPI process and provide a physical picture of the control mechanism. To validate the model, the results are compared to an ab initio calculation based on the solution of the two-dimensional time-dependent Schr\"odinger equation for the nonperturbative interaction of an atom with intense polarization-shaped bichromatic femtosecond-laser pulses. Our results indicate that the control mechanism is robust with respect to the laser intensity, facilitating its experimental observation.
In this paper, we theoretically demonstrate that the (2+1+1) resonance enhanced multi-photon ionization photoelectron spectroscopy in sodium atom can be effectively controlled by shaping femtosecond laser pulse with a π phase step modulation in weak laser field, involving its total photoelectron energy, maximal photoelectron intensity, and spectroscopic bandwidth. Our results show that the total photoelectron energy can be suppressed but not enhanced, the maximal photoelectron intensity can be enhanced and also suppressed, and the photoelectron spectroscopy can be tremendously narrowed. These theoretical results can provide a feasible scheme to achieve the high-resolution photoelectron spectroscopy and study the excited state structure in atomic and molecular systems.