Nonlinear vortex dichroism in chiral molecules

TL;DR

This paper introduces the theory of nonlinear vortex dichroism in chiral molecules, revealing new ways to probe molecular chirality using focused optical vortices in two-photon absorption processes.

Contribution

It presents a novel theoretical framework for two-photon absorption of focused vortex beams by chiral molecules, highlighting unique features and potential applications in chiroptical spectroscopy.

Findings

Distinct features in TPA with vortex beams enable probing of molecular structure.

Differential TPA rate is affected by linear polarization orientation.

Nonlinear optical activity combined with structured light offers new chiral analysis methods.

Abstract

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.