Limits of the Plane Wave Approximation in the Measurement of Molecular Properties

TL;DR

This paper examines the limitations of the plane wave approximation in molecular tomography, demonstrating how wavefunction distortions impact the accuracy of reconstructed molecular orbitals using high harmonic spectra.

Contribution

It provides an analysis of how scattering wavefunction distortions influence molecular orbital reconstructions, highlighting the approximation's limitations in ultrafast molecular property measurements.

Findings

Distortions significantly affect orbital reconstructions

Plane wave approximation validity depends on molecular context

Implications for ultrafast molecular imaging accuracy

Abstract

Rescattering electrons offer great potential as probes of molecular properties on ultrafast timescales. The most famous example is molecular tomography, in which high harmonic spectra of oriented molecules are mapped to ``tomographic images'' of the relevant molecular orbitals. The accuracy of such reconstructions may be greatly affected by the distortion of scattering wavefunctions from their asymptotic forms due to interactions with the parent ion. We investigate the validity of the commonly used plane wave approximation in molecular tomography, showing how such distortions affect the resulting orbital reconstructions.