Optical-pumping enantio-conversion of chiral mixtures in presence of tunneling between chiral states

TL;DR

This paper proposes an optical-pumping scheme for enantio-conversion of chiral molecules that accounts for tunneling interactions between chiral states, achieving high efficiency through careful electromagnetic field design.

Contribution

It introduces a novel four-level model including tunneling interactions and demonstrates a method to selectively convert chiral states using optical pumping.

Findings

High-efficiency enantio-conversion achieved numerically

Tunneling interactions can be effectively managed

Selective excitation of chiral states demonstrated

Abstract

Enantio-conversion of chiral mixtures, converting the mixtures composed of left- and right-handed chiral molecules into the homochiral ensembles, has become an important research topic in chemical and biological fields. In previous studies on enantio-conversion, the tunneling interaction between the left- and right-handed chiral states was often neglected. However, for certain chiral molecules, this tunneling interaction is significant and cannot be ignored. Here we propose a scheme for enantio-conversion of chiral mixtures through optical pumping based on a four-level model of chiral molecules, comprising two chiral ground states and two achiral excited states, with a tunneling interaction between the chiral states. Under one-photon large detuning and two-photon resonance conditions, one of the achiral excited states is eliminated adiabatically. By well designing the detuning and coupling strengths of the electromagnetic fields, the tunneling interaction between two chiral states and the interaction between one of the chiral states and the remaining achiral excited state can be eliminated. Consequently, one chiral state remains unchanged, while the other can be excited to an achiral excited state, establishing chiral-state-selective excitations. By numerically calculating the populations of two chiral ground states and the enantiomeric excess, we observe that high-efficiency enantio-conversion is achieved under the combined effects of system dissipation and chiral-state-selective excitations.