Multiple orbital contributions to molecular high-harmonic generation in an asymmetric top

TL;DR

This study demonstrates that high-harmonic generation in asymmetric top molecules involves multiple orbitals, with spectral features depending on molecular axis and harmonic order, enabling orbital-specific probing.

Contribution

It reveals that multiple orbitals contribute to HHG in asymmetric top molecules, expanding understanding beyond linear molecules and suggesting new probing techniques.

Findings

Spectral features depend on molecular axis and harmonic order.

Multiple orbitals contribute to HHG in asymmetric top molecules.

HHG can be used to probe orbital dependencies in asymmetric molecules.

Abstract

High-order harmonic generation (HHG) in aligned linear molecules can offer valuable information about strong-field interactions in lower-lying molecular orbitals, but extracting this information is difficult for three-dimensional molecular geometries. Our measurements of the asymmetric top SO2 show large axis dependencies, which change with harmonic order. The analysis shows that these spectral features must be due to field ionization and recombination from multiple orbitals during HHG. We expect that HHG can probe orbital dependencies using this approach for a broad class of asymmetric-top molecules.