Molecular orbital tomography of HOMO and HOMO-1 of the nonlinear molecule H2O: The study on multi-orbital effects

Abstract

Molecular orbital tomography (MOT) through high-order harmonic generation (HHG) is a crucial method for probing individual molecular orbitals. Previous studies mainly focused on linear molecules such as N2, and CO, where valence orbitals were imaged by detecting harmonic emission at various alignments. In this study, we investigate the HHG from the water molecules, with the aim of exploring MOT for nonlinear molecules. By employing the time-dependent density functional theory, we obtain HHG spectra for different angles between the laser polarization and molecular symmetry axis. By manipulating the scanning planes (planes perpendicular to the laser propagation direction and contain the field polarization direction), specific orbitals can be selectively imaged. Particularly, a well-reconstructed highest occupied molecular orbital (HOMO) is obtained when the laser scanning plane approximately aligns with the nodal plane of HOMO-1. However, when the laser polarization deviates from the nodal plane, multiple orbitals contribute to the HHG process, and we visualize the orbital distortions resulting from such effects. Furthermore, HOMO-1, can be reconstructed when the laser scanning plane aligns with the nodal plane of HOMO. This research significantly advances the development of MOT and opens up intriguing possibilities for reconstructing orbitals of more complex molecules.