Nonlinear vortex dichroism in chiral molecules

Fuente: arXiv
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Autori principali: Cheeseman, Luke, Forbes, Kayn A
Natura: Preprint
Pubblicazione: 2024
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author Cheeseman, Luke
Forbes, Kayn A
author_facet Cheeseman, Luke
Forbes, Kayn A
contents The recent discovery that linearly polarized light with a helical wavefront can exhibit vortex dichroism (also referred to as helical dichroism) has opened up new horizons in chiroptical spectroscopy with structured chiral light. Recent experiments have now pushed optical activity with vortex beams into the regime of nonlinear optics. Here we present the theory of two-photon absorption (TPA) of focused optical vortices by chiral molecules: nonlinear vortex dichroism (NVD). We discover that highly distinct features arise in the case of TPA with focused vortex beams, including the ability to probe chiral molecular structure not accessible to current methods and that the differential rate of TPA is significantly influenced by the orientation of the state of linear polarization. This work provides strong evidence that combining nonlinear optical activity with structured light provides new and improved routes to studying molecular chirality.
format Preprint
id arxiv_https___arxiv_org_abs_2408_05994
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Nonlinear vortex dichroism in chiral molecules
Cheeseman, Luke
Forbes, Kayn A
Optics
Chemical Physics
The recent discovery that linearly polarized light with a helical wavefront can exhibit vortex dichroism (also referred to as helical dichroism) has opened up new horizons in chiroptical spectroscopy with structured chiral light. Recent experiments have now pushed optical activity with vortex beams into the regime of nonlinear optics. Here we present the theory of two-photon absorption (TPA) of focused optical vortices by chiral molecules: nonlinear vortex dichroism (NVD). We discover that highly distinct features arise in the case of TPA with focused vortex beams, including the ability to probe chiral molecular structure not accessible to current methods and that the differential rate of TPA is significantly influenced by the orientation of the state of linear polarization. This work provides strong evidence that combining nonlinear optical activity with structured light provides new and improved routes to studying molecular chirality.
title Nonlinear vortex dichroism in chiral molecules
topic Optics
Chemical Physics
url https://arxiv.org/abs/2408.05994