Electron correlation effects in enhanced-ionization of molecules:A time-dependent generalized-active-space configuration-interaction study

TL;DR

This study investigates how electron correlation influences enhanced ionization in molecules like H2 and LiH using advanced time-dependent configuration-interaction methods, revealing significant correlation effects and phase-dependent phenomena.

Contribution

It introduces a detailed analysis of correlation effects in enhanced ionization using the time-dependent generalized-active-space configuration-interaction approach, highlighting deviations from single-electron models.

Findings

Enhanced ionization occurs in multielectron molecules.

Correlation significantly affects ionization dynamics.

Carrier-envelope-phase strongly influences ionization in asymmetric molecules.

Abstract

We numerically study models of $\mathrm{H}_2$ and $\mathrm{LiH}$ molecules, aligned collinearly with the linear polarization of the external field, to elucidate the possible role of correlation in the enhanced-ionization phenomena. Correlation is considered at different levels of approximation with the time-dependent generalized-active-space configuration-interaction method. The results of our studies show that enhanced ionization occurs in multielectron molecules, that correlation is important and they also demonstrate significant deviations between the results of the single-active-electron approximation and more accurate configuration-interaction methods. With the inclusion of correlation we show strong carrier-envelope-phase effects in the enhanced ionization of the asymmetric heteronuclear $\mathrm{LiH}$-like molecule. The correlated calculation shows an intriguing feature of cross-over in enhanced ionization with two carrier-envelope-phases at critical inter-nuclear separation.