Theory of angular momentum transfer from light to molecules

Fuente: arXiv
Saved in:
Bibliographic Details
Main Authors: Maslov, Mikhail, Koutentakis, Georgios M., Hrast, Mateja, Heckl, Oliver H., Lemeshko, Mikhail
Format: Preprint
Published: 2023
Subjects:
Online Access:
Tags: Add Tag
No Tags, Be the first to tag this record!
_version_ 1866916465205051392
author Maslov, Mikhail
Koutentakis, Georgios M.
Hrast, Mateja
Heckl, Oliver H.
Lemeshko, Mikhail
author_facet Maslov, Mikhail
Koutentakis, Georgios M.
Hrast, Mateja
Heckl, Oliver H.
Lemeshko, Mikhail
contents We present a theory describing interaction of structured light, such as light carrying orbital angular momentum, with molecules. The light-matter interaction Hamiltonian we derive is expressed through couplings between spherical gradients of the electric field and the (transition) multipole moments of a particle of any non-trivial rotation point group. Our model can therefore accommodate for an arbitrary complexity of the molecular and electric field structure, and can be straightforwardly extended to atoms or nanostructures. Applying this framework to ro-vibrational spectroscopy of molecules, we uncover the general mechanism of angular momentum exchange between the spin and orbital angular momenta of light, molecular rotation and its center-of-mass motion. We show that the non-zero vorticity of Laguerre-Gaussian beams can strongly enhance certain ro-vibrational transitions that are considered forbidden in the case of non-helical light. We discuss the experimental requirements for the observation of these forbidden transitions in state-of-the-art spatially-resolved spectroscopy measurements.
format Preprint
id arxiv_https___arxiv_org_abs_2310_00095
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Theory of angular momentum transfer from light to molecules
Maslov, Mikhail
Koutentakis, Georgios M.
Hrast, Mateja
Heckl, Oliver H.
Lemeshko, Mikhail
Atomic Physics
Atomic and Molecular Clusters
Chemical Physics
Optics
We present a theory describing interaction of structured light, such as light carrying orbital angular momentum, with molecules. The light-matter interaction Hamiltonian we derive is expressed through couplings between spherical gradients of the electric field and the (transition) multipole moments of a particle of any non-trivial rotation point group. Our model can therefore accommodate for an arbitrary complexity of the molecular and electric field structure, and can be straightforwardly extended to atoms or nanostructures. Applying this framework to ro-vibrational spectroscopy of molecules, we uncover the general mechanism of angular momentum exchange between the spin and orbital angular momenta of light, molecular rotation and its center-of-mass motion. We show that the non-zero vorticity of Laguerre-Gaussian beams can strongly enhance certain ro-vibrational transitions that are considered forbidden in the case of non-helical light. We discuss the experimental requirements for the observation of these forbidden transitions in state-of-the-art spatially-resolved spectroscopy measurements.
title Theory of angular momentum transfer from light to molecules
topic Atomic Physics
Atomic and Molecular Clusters
Chemical Physics
Optics
url https://arxiv.org/abs/2310.00095