Optically Addressing Circularly-Polarized Vibrations in Molecules

TL;DR

This paper investigates how symmetry-breaking chemical modifications influence the ability to optically address circularly-polarized vibrations in molecules, revealing broader possibilities for using these vibrations in nanoscale information applications.

Contribution

It demonstrates that certain molecules can retain CP vibrational modes despite symmetry-breaking, expanding potential applications beyond non-Abelian symmetry molecules.

Findings

CP vibrations can be optically addressed in molecules with broken symmetry.

Some vibrational modes remain degenerate and orthogonal after modifications.

Potential for experimental CP pump-probe techniques is discussed.

Abstract

Circularly-polarized (CP) vibrations are the nuclear-motion analog of CP light, emerging in molecules with non-Abelian point-group symmetry that support orthogonal and degenerate vibrational normal modes. Here, we explore the optical addressability of CP vibrations, motivated by their potential as nanoscale angular momentum states suitable for information storage and manipulation. We investigate how symmetry-breaking chemical modifications affect a molecule's capacity to support CP vibrations. Notably, we find cases where modes retain their orthogonality and degeneracy in spite of such modifications, broadening the opportunities afforded by CP vibrations beyond non-Abelian point-group molecules. Prospects for experimental implementations using CP pump-probe techniques are briefly discussed.