Vibrational interference of Raman and high-harmonic generation pathways

TL;DR

This paper introduces a model explaining how molecular vibrational states interfere during high harmonic generation, affecting light intensity, and develops a semiclassical electron propagation model linked to electron-ion scattering.

Contribution

It provides a novel interference-based explanation for vibrational effects in high harmonic generation and introduces a semiclassical model connecting electron propagation with scattering.

Findings

Vibrational states modulate harmonic intensity through interference.

A semiclassical model links electron propagation with scattering.

The model aligns with experimental observations.

Abstract

Experiments have shown that the internal vibrational state of a molecule can affect the intensity of high harmonic light generated from that molecule. This paper presents a model which explains this modulation in terms of interference between different vibrational states occurring during the high harmonic process. In addition, a semiclassical model of the continuum electron propagation is developed which connects with rigorous treatments of the electron-ion scattering.