High-Order Harmonic Generation and Molecular Orbital Tomography: Characteristics of Molecular Recollision Electronic Wave Packets

TL;DR

This paper explores how molecular orientation affects high-order harmonic generation and reveals that molecular recollision electronic wave packets are influenced by ionization potential and orbital origin, impacting molecular orbital tomography.

Contribution

It provides a detailed analysis of the orientation dependence of molecular HHG and characterizes the properties of molecular recollision electronic wave packets.

Findings

REWPs depend on ionization potential and orbital origin

Spectral amplitude varies due to interference between atomic cores

Implications for molecular orbital tomography accuracy

Abstract

We investigate the orientation dependence of molecular high-order harmonic generation (HHG) both numerically and analytically. We show that the molecular recollision electronic wave packets (REWPs) in the HHG are closely related to the ionization potential as well as the particular orbital from which it ionized. As a result, the spectral amplitude of the molecular REWP can be significantly different from its reference atom (i.e., with the same ionization potential as the molecule under study) in some energy regions due to the interference between the atomic cores of the molecules. This finding is important for molecular orbital tomography using HHG[Nature \textbf{432}, 867(2004)].