Study of laser-driven multielectron dynamics of Ne atom using time-dependent optimized second-order many-body perturbation theory

TL;DR

This paper introduces a time-dependent optimized second-order many-body perturbation theory (TD-OMP2) for simulating multielectron dynamics in neon atoms under intense laser fields, demonstrating its stability and moderate accuracy compared to other methods.

Contribution

The paper develops and applies the TD-OMP2 method for strong-field atomic dynamics, showing its advantages over TD-CC2 and TDHF in stability and suitability for large systems.

Findings

TD-OMP2 overestimates Ne response, TDHF underestimates it

TD-CC2 is unstable at high intensities and non-gauge-invariant

TD-OMP2 enables stable simulation of nonlinear phenomena

Abstract

We calculate the high-harmonic generation (HHG) spectra, strong-field ionization, and time-dependent dipole-moment of Ne using explicitly time-dependent optimized second-order many-body perturbation method (TD-OMP2) where both orbitals and amplitudes are time-dependent. We consider near-infrared (800 nm) and mid-infrared (1200 nm) laser pulses with very high intensities ($5\times10^{14}$, $8\times10^{14}$ , and $1\times10^{15}$ W/cm$^2$), required for strong-field experiments with the high-ionization potential (21.6 eV) atom. We compare the result of the TD-OMP2 method with the time-dependent complete-active-space self-consistent field method and the time-dependent Hartree-Fock method. Further, we report the implementation of the TD-CC2 method within the chosen active space, which is also a second-order approximation to the TD-CCSD method, and present results of time-dependent dipole-moment and HHG spectra with an intensity of $5\times10^{13}$ W/cm$^2$ at a wavelength of 800 nm. It is found that the TD-CC2 method is not stable in the case with a higher laser intensity, and it does not provide a gauge-invariant description of the physical properties, which makes TD-OMP2 a superior choice to reach out to larger chemical systems, especially for the study of strong-field dynamics. The obtained results indicate that the TD-OMP2 method shows moderate performance, overestimating the response of Ne, while TDHF underestimates it. Nevertheless, it is remarkable that stable computation of such highly nonlinear nonperturbative phenomena is possible within the framework of time-dependent perturbation method, by virtue of the nonperturbative inclusion of the laser-electron interaction and time-dependent optimization of orbitals.