Interaction between vortex beams and diatomic molecules with rotation

TL;DR

This paper develops a theoretical framework to analyze how vortex beams interact with diatomic molecules, especially considering molecular rotation, revealing new angular momentum transfer mechanisms and transition pathways.

Contribution

It introduces a spherical harmonics-based theoretical model incorporating molecular rotation and demonstrates how vortex beams induce specific rotational transitions in diatomic molecules.

Findings

Vortex beams can carry angular momentum of 0, ħ, or 2ħ.

The model predicts selection rules for rotational transitions.

Vortex beams offer new methods for molecular state control.

Abstract

The interaction between vortex beam (VB) and molecule has drawn much attention in recent years, but the lack of theoretical method somehow limits its further analysis, especially when the molecular rotational degree of freedom is involved and coupled with the molecular electronic states. To incorporate the molecular rotation into the theoretical study, in this paper, we describe the diatomic molecular states in Hund's coupling basis and express interaction Hamiltonian in form of spherical harmonics expansion, and then investigate the rotational transition of molecular states driven by VB. The theory clearly illustrates that each photon of VB may carry a total angular momentum of 0, $\hbar$, or 2$\hbar$, and therefore could drive O, P, Q, R and S branches of diatomic molecular rotational transitions with some specific selection rules. These results indicate that VB could provide new methods for preparing and measuring the diatomic molecular states.