Orientational decomposition of molecular high harmonic emission in three dimensions

TL;DR

This paper introduces a method to analyze high harmonic generation in asymmetric top molecules, enabling 3D structural insights and expanding the applicability of HHG-based molecular imaging.

Contribution

It presents a novel approach to extract orientation-dependent information from asymmetric tops, extending HHG tomography into three dimensions for complex molecules.

Findings

Successfully decomposed HHG signals from SO2

Extended HHG tomography to three dimensions

Demonstrated potential for probing electron dynamics in complex molecules

Abstract

An important goal in molecular physics and chemistry today is to obtain structure-dependent information about molecular function to obtain a deeper understanding into chemical reactions. However, until now, asymmetric tops, which comprise the widest and most general class of molecules, remain principally unexplored. This gap is particularly evident in high harmonic generation (HHG). HHG has successfully obtained structural information about electron hole pairs or orbitals for simple linear molecules. Unfortunately, for more complicated molecules, the emission from different molecular directions interfere, concealing individual angular signatures. Here we introduce a method to extract orientation-dependent information from asymmetric tops and apply it to the sulfur dioxide (SO2) molecule. We use the rotational revival structure to decompose the angular contributions of HHG emission. This method also extends HHG-based tomographic imaging into three dimensions and makes it applicable to a much wider class of systems than previously envisioned. Our results suggest that HHG is a powerful tool to probe electron orbital structure and dynamics of complex molecules.