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Enantio-conversion of chiral mixtures, converting the mixtures composed ofleft- and right-handed chiral molecules into the homochiral ensembles, hasbecome an important research topic in chemical and biological fields. Inprevious studies on enantio-conversion, the tunneling interaction between theleft- and right-handed chiral states was often neglected. However, for certainchiral molecules, this tunneling interaction is significant and cannot beignored. Here we propose a scheme for enantio-conversion of chiral mixturesthrough optical pumping based on a four-level model of chiral molecules,comprising two chiral ground states and two achiral excited states, with atunneling interaction between the chiral states. Under one-photon largedetuning and two-photon resonance conditions, one of the achiral excited statesis eliminated adiabatically. By well designing the detuning and couplingstrengths of the electromagnetic fields, the tunneling interaction between twochiral states and the interaction between one of the chiral states and theremaining achiral excited state can be eliminated. Consequently, one chiralstate remains unchanged, while the other can be excited to an achiral excitedstate, establishing chiral-state-selective excitations. By numericallycalculating the populations of two chiral ground states and the enantiomericexcess, we observe that high-efficiency enantio-conversion is achieved underthe combined effects of system dissipation and chiral-state-selectiveexcitations.

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