Above-Threshold Ionization and Laser-Induced Electron Diffraction in Diatomic Molecules

TL;DR

This paper develops an analytic theoretical model for strong field ionization and electron diffraction in diatomic molecules, enabling better understanding of molecular dynamics with laser interactions and matching experimental results.

Contribution

It introduces a generalized strong field approximation with an analytic solution that accurately models electron emission and diffraction in diatomic molecules, free from gauge-dependent issues.

Findings

Analytic expressions match numerical TDSE results for H₂⁺.

Model successfully reproduces experimental LIED features for O₂⁺.

Approach is extendable to complex molecules and multi-electron systems.

Abstract

Strong field photoemission and electron recollision provide a viable route to extract electronic and nuclear dynamics from molecular targets with attosecond temporal resolution. However, since an {\em ab-initio} treatment of even the simplest diatomic systems is beyond today's capabilities approximate qualitative descriptions are warranted. In this paper, we develop such a theoretical approach to model the photoelectrons resulting from intense laser-molecule interaction. We present a general theory for symmetric diatomic molecules in the single active electron approximation that, amongst other capabilities, allows adjusting both the internuclear separation and molecular potential in a direct and simple way. More importantly we derive an analytic approximate solution of the time dependent Schr\"odinger equation (TDSE), based on a generalized strong field approximation (SFA) version. Using that approach we obtain expressions for electrons emitted transition amplitudes from two different molecular centres, and accelerated then in the strong laser field. One innovative aspect of our theory is the fact that the dipole matrix elements are free from non-physical gauge and coordinate system dependent terms -- this is achieved by adapting the coordinate system, in which SFA is performed, to the centre from which the corresponding part of the time dependent wave function originates. Our analytic results agree very well with the numerical solution of the full three-dimensional TDSE for the H$_2^+$ molecule. Moreover, the theoretical model was applied to describe laser-induced electron diffraction (LIED) measurements of O$_2^+$ molecules, obtained at ICFO, and reproduces the main features of the experiment very well. Our approach can be extended in a natural way to more complex molecules and multi-electron systems.