Quantum Dynamics of Enantiomers in Chiral Optical Cavities

TL;DR

This paper presents a theoretical framework showing that chiral optical cavities under strong coupling can induce enantioselective effects, enabling detection and control of molecular handedness through cavity-induced energy shifts and spectroscopic signatures.

Contribution

The work introduces a novel quantum electrodynamics model demonstrating cavity-induced enantioselectivity and proposes ultrafast spectroscopy for experimental detection.

Findings

Cavity field lifts degeneracy of enantiomers at the electronic level.

Strong coupling creates enantioselective polariton states.

Simulated 2DES spectra reveal enantioselective signatures.

Abstract

Chirality, the absence of mirror symmetry, is a fundamental molecular property with far-reaching consequences from chemistry to biology. Yet enantiosensitive optical responses are very weak. Here, we introduce a theoretical framework in which a chiral optical cavity under strong coupling directly lifts the degeneracy of opposite enantiomers at the electronic-dipole level. The cavity's parity-breaking field inside the cavity induces distinct site-energy shifts for left- versus right-handed molecules, producing robust enantioselective polariton states that overcome the weakness of traditional chiroptical effects. Using cavity quantum electrodynamics simulations, we show that strong light-matter coupling reshapes the polaritonic energy landscape and leads to enantiomer-specific coherence lifetimes and relaxation pathways. To reveal these dynamics, we propose ultrafast two-dimensional electronic spectroscopy (2DES) as a probe, capable of resolving polaritonic splittings on femtosecond timescales. Simulated 2DES spectra exhibit unambiguous enantioselective signatures of the cavity-induced asymmetry. These findings establish that chiral cavities provide a powerful platform for detecting and controlling molecular handedness beyond the limits of conventional optical methods.