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Chinese Physics B

Wavelength- and ellipticity-dependent photoelectron spectra from multiphoton ionization of atoms

Keyu Guo, Min Li, Jintai Liang, Chuanpeng Cao, Yueming Zhou, Peixiang Lu

Published Oct 19, 2022• 3 citations
Publisher

Abstract

We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Schrödinger equation. The photoelectron momentum distributions display many ring-like patterns for the three-photon ionization, which vary dramatically with the change of the laser wavelength. We show that the wavelength-dependent photoelectron energy spectrum can be used to effectively identify the resonant and nonresonant ionization pathways. We also find an abnormal ellipticity dependence of the electron yield for the (2+1) resonance-enhanced ionization via the 4d intermediate state, which is relevant to the two-photon excitation probability from the ground state to the 4d state.

DOI
10.1088/1674-1056/ac9b36

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We theoretically study the photoelectron momentum distributions from multiphoton ionization of a model lithium atom over a range of laser wavelengths from 500 nm to 700 nm by numerically solving the time-dependent Schrödinger equation. The photoelectron momentum distributions display many ring-like patterns for the three-photon ionization, which vary dramatically with the change of the laser wavelength. We show that the wavelength-dependent photoelectron energy spectrum can be used to effectively identify the resonant and nonresonant ionization pathways. We also find an abnormal ellipticity dependence of the electron yield for the (2+1) resonance-enhanced ionization via the 4d intermediate state, which is relevant to the two-photon excitation probability from the ground state to the 4d state.
We calculate two-dimensional photoelectron momentum distributions and energy spectra after multiphoton ionization of Li atoms subject to intense laser fields in the one-photon Rabi-flopping regime. The time-dependent Schr\"odinger equation is solved within the single-active-electron approximation using a model potential which reproduces accurately the binding energies and dipole matrix elements of the Li atom. Interaction with the external electromagnetic field is treated within the dipole approximation. We show that the Rabi oscillations of the population between the ground 2s2s2s state and the excited 2p2p2p state in the one-photon resonance regime are reflected in the energy spectra of emitted photoelectrons, which manifest interference structures with minima. Transformations of the interference structures in the photoelectron energy spectra caused by the variation of the laser peak intensity and pulse duration are analyzed.
We present experimental and theoretical data on the electron energy spectra from resonance-enhanced multiphoton ionization of atoms. In experiments performed with 594-nm wavelength, linearly polarized laser pulses of 300-fs and 600-fs durations, it is found that excitation of the intermediate resonances during the rising edge of the laser pulse can dominate the electron spectrum. Good agreement is found between the experimental results and a model based on the Landau-Zener energy level crossing theory. Theoretical results obtained with direct integration of the Schrödinger equation show that intermediate resonances can be excited appreciably off resonance if the coupling between the ground state and the excited state is highly nonlinear. The excitation of the intermediate state is not localized at the intensity which makes it six-photon resonant with the ground state. A multilevel model used to simulate the experimental spectra, based on direct integration of the Schrödinger equation, shows excellent agreement with the data.
A joint experimental and theoretical study of four-photon ionization of Li is performed using a pump-probe setup with the laser frequency tuned in between the excitation energies of the 2s2s2s--4p4p4p and 2s2s2s--4f4f4f three-photon transitions. The three-dimensional photoelectron momentum pattern is recorded as a function of the delay time between two otherwise identical laser pulses. The process is modeled by numerically solving the time-dependent Schr\"odinger equation. While complicated interference patterns arise in the electron spectrum when the two pulses partially overlap in time, the expected quantum-beat phenomenon between Li atoms in either the 4p4p4p or the 4f4f4f state are seen when the fast oscillations involving the 2s2s2s initial state are averaged over. The qualitative agreement between the predicted and observed beating patterns is very good.
We present both experimental and theoretical studies of resonantly enhanced multiphoton ionization of cesium atoms. Photoelectron angular distributions for two-photon ionization via the one-photon-allowed 7p2P12,327p^{2}P_{\frac{1}{2},\frac{3}{2}}7p2P21​,23​​ and 8p2P12,328p^{2}P_{\frac{1}{2},\frac{3}{2}}8p2P21​,23​​ intermediate states and three-photon ionization via the two-photon-allowed 8d2D52,328d^{2}D_{\frac{5}{2},\frac{3}{2}}8d2D25​,23​​ resonant intermediate states are reported. The photoelectrons are energy analyzed with a spherical-sector electrostatic energy analyzer with an energy resolution of ~ 0.1 eV and angular resolution of ~ \ifmmode\pm\else\textpm\fi{}2\ifmmode^\circ\else\textdegree\fi{}. A straightforward calculation based upon a finestructure scheme gives excellent agreement with the measured angular distributions for the 2P12^{2}P_{\frac{1}{2}}2P21​​ states. The laser pulse duration is comparable to the hyperfine precession period which allows the hyperfine coupling to partially destroy the anisotropy initially produced in the 2P32^{2}P_{\frac{3}{2}}2P23​​ resonant intermediate states. Quantitative calculations including hyperfine coupling take this into account and provide an expression which gives a reasonable fit to the 2P32^{2}P_{\frac{3}{2}}2P23​​ data.
A theoretical investigation has been carried out on the dependence of the photoelectron angular distributions on laser intensity for the case of two-photon-resonant three-photon ionization of sodium. Good overall agreement is obtained with the experimental anisotropy parameters for ionization via the 4D3/2{D}_{3/2}D3/2​ and 4D5/2{D}_{5/2}D5/2​ intermediate states. The comparison of the theoretical results with the experimental data also clearly shows that the hyperfine splitting of the ground state has to be taken into account at high laser intensities although the low-intensity angular distributions do not depend on the initial ground hyperfine state.
We measure photoion spectra and angular distributions of photoelectrons from the two-color, two-photon resonant ionization of barium atoms in order to probe the effect of the photoionization pathway on autoionization processes. The (6s6p)1{)}^{1})1P${\mathrm{\ifmmode^\circ\else\textdegree\fi{}}}_{1}$ and the (5d6p)1{)}^{1})1P${\mathrm{\ifmmode^\circ\else\textdegree\fi{}}}_{1}$ states are used as intermediates in the photoexcitation of barium to energies in the range of a series of 5dnd autoionizing states. Dramatic differences in the profiles of autoionizing lines are observed for excitation pathways involving different intermediate states. Angular distributions of photoelectrons collected across the range of autoionizing resonances demonstrate strong variations that follow constraints imposed by the angular momentum of the autoionizing peaks and also suggest significant spin-orbit interactions in the photoionization step.