Twisted Raman: Orbital Angular Momentum Control of Raman Optical Activity

Forbes, Kayn A. ORCID: https://orcid.org/0000-0002-8884-3496 (2026) Twisted Raman: Orbital Angular Momentum Control of Raman Optical Activity. The Journal of Physical Chemistry Letters, 17. pp. 10682-10690. ISSN 1948-7185

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Abstract

Raman optical activity (ROA) conventionally detects differences in Raman scattering associated with opposite circular-polarization states σ, providing a sensitive probe of molecular chirality. Here we show that a different handedness of light can drive ROA: the wavefront handedness encoded in the topological charge l of a focused optical vortex. Instead of using photons carrying spin angular momentum σℏ, the response is controlled by photons carrying orbital angular momentum lℏ, with the sign of l defining the optical handedness. We develop a nonparaxial theory of ROA with Laguerre−Gaussian beams and show that the Maxwell-consistent focused field allows a linearly polarized vortex beam to produce a topological-charge-dependent ROA signal from an isotropic ensemble of independent, randomly oriented chiral molecules, as in a gas or dilute solution. The response contains both electric-dipole−magnetic-dipole and electric-dipole−electric-quadrupole interference terms, establishing optical orbital angular momentum as a control parameter for chiral Raman spectroscopy.

Item Type:	Article
Faculty \ School:	Faculty of Science > School of Chemistry, Pharmacy and Pharmacology
UEA Research Groups:	Faculty of Science > Research Groups > Physical Chemistry and Pharmaceutics
Depositing User:	LivePure Connector
Date Deposited:	21 Sep 2026 08:45
Last Modified:	21 Sep 2026 08:45
URI:	https://ueaeprints.uea.ac.uk/id/eprint/104594
DOI:	issn:1948-7185

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