Molecular Orbital Tomography using Short Laser Pulses

TL;DR

This paper demonstrates that molecular orbital tomography using high harmonic generation is feasible with extremely short laser pulses, introducing a new reconstruction method based on momentum matrix elements and validating it through simulations.

Contribution

It introduces a novel approach for molecular orbital tomography with short laser pulses using momentum matrix elements, expanding the applicability of the technique.

Findings

Reconstruction is possible with short laser pulses.

A new equation based on momentum matrix elements is proposed.

Simulations validate the effectiveness of the method.

Abstract

Recently, a method to image molecular electronic wave functions using high harmonic generation (HHG) was introduced by Itatani \textit{et al.\} [Nature {\textbf{432}}, 876 (2004)]. We show that, while the tomographic reconstruction of general orbitals with arbitrary symmetry cannot be performed with long laser pulses, this becomes possible when extremely short pulses are used. An alternative reconstruction equation based on momentum matrix elements, rather than on dipole matrix elements, is proposed. We present simulations of the procedure for 2D model systems based on numerical solutions of the time-dependent Schr\"{o}dinger equation, and present results from further post-processing of the reconstructed orbitals.