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Spin polarization in the multiphoton above-threshold ionization of 5p3/2- and 5p1/2-electrons of Xe with intense 395nm, circularly polarized laser pulses, is investigated theoretically. For this purpose, we solve the time-dependent Schrödinger equation on the basis of spherical spinors. We, thus, simultaneously propagate the spin-up and spin-down single-active-electron wave packets, driven by the laser pulses in the ionic potential, which includes the spin–orbit interaction explicitly. The present theoretical results are in good agreement with the recent experimental results [D. Trabert et al., Phys. Rev. Lett. 120, 043202 (2018)]. [ABSTRACT FROM AUTHOR]

Photoelectron circular dichroism (PECD) in different regimes of multiphoton ionization of fenchone is studied theoretically using the time-dependent single center method. In particular, we investigate the chiral response to the one-color multiphoton or strong-field ionization by circularly polarized 400 nm and 814 nm optical laser pulses or 1850 nm infrared pulse. In addition, the broadband ionization by short coherent circularly polarized 413–1240 nm spanning pulse is considered. Finally, the two-color ionization by the phase-locked 400 nm and 800 nm pulses, which are linearly polarized in mutually orthogonal directions, is investigated. The present computational results on the one-color multiphoton ionization of fenchone are in agreement with the available experimental data. For the ionization of fenchone by broadband and bichromatic pulses, the present theoretical study predicts substantial multiphoton PECDs. [ABSTRACT FROM AUTHOR]

A theoretical method to study the angle-resolved multiphoton ionization of polyatomic molecules is developed. It is based on the time-dependent formulation of the Single Center (TDSC) method and consists in the propagation of single-active-electron wave packets in the effective molecular potentials in the presence of intense laser pulses. For this purpose, the time-dependent Schrödinger equation for one electron, moving in a molecular field and interacting with an arbitrary laser pulse, is solved in spherical coordinates by an efficient numerical approach. As a test, the method is applied to the one- and two-photon ionizations of a model methane-like chiral system by circularly polarized short intense high-frequency laser pulses. Thereby, we analyze the photoelectron circular dichroism (PECD) in the momentum distribution. The considered model application illustrates the capability of the TDSC method to study multiphoton PECD in fixed-in-space and randomly oriented chiral molecules. [ABSTRACT FROM AUTHOR]

Using a model methanelike chiral system, we theoretically demonstrate a possibility to access photoelectron circular dichroism (PECD) by a single experiment with two overlapping laser pulses of carrier frequencies ω and 2ω, which are linearly polarized in two mutually orthogonal directions. Depending on the relative phase, the resulting electric field can be tailored to have two different rotational directions in the upper and lower hemispheres along the polarization of the ω pulse. We predict a strong forward-backward asymmetry in the emission of photoelectrons from randomly oriented samples, which has an opposite sign in the upper and lower hemispheres. The predicted PECD effect is phase and enantiomer sensitive, providing new insight in this fascinating fundamental phenomenon. The effect can be optimized by varying relative intensities of the pulses. [ABSTRACT FROM AUTHOR]

Photoionization of the hydrogen atom by intense and short coherent laser pulses is investigated from first principles by a numerical solution of the time-dependent Schrödinger equation in the dipole-velocity gauge. The considered photon energies are resonant to the 1 s → 2 p excitation, and the pulse intensities are high enough to induce Rabi floppings. The computed resonance-enhanced two-photon ionization spectra as well as the three-photon above threshold ionization spectra exhibit pronounced multiple-peak patterns due to dynamic interference. Fingerprints of dynamic interference can also be seen directly in the radial density of the photoelectron. The impact of the variation of the pulse intensity and photon energy on the dynamic interference is investigated, and the angular distribution of the emitted electrons is analyzed in some details. The present precise numerical results confirm our previous theoretical predictions on the two-photon ionization spectra (Demekhin and Cederbaum, 2012) made within a minimal few-level model. [ABSTRACT FROM AUTHOR]