Evading thermal population influence in enantiomeric-specific state transfer based on a cyclic three-level system via ro-vibrational transitions

Abstract

Optical methods of enantiomeric-specific state transfer had been proposed theoretically based on a cyclic three-level system of chiral molecule. According to these theoretical methods, recently the breakthrough progress has been reported in experiments [S. Eibenberger et al., Phys. Rev. Lett. 118, 123002 (2017); C. Pérez et al., Angew. Chem. Int. Ed. 56, 12512 (2017)] for cold gaseous chiral molecules but with low state-specific enantiomeric enrichment. One of the limiting factors is the influence of the thermal population in the selected three purely rotational states in experiment. Here, we theoretically propose an improved optical method of enantiomeric-specific state transfer to effectively evade such an adverse impact of thermal population by introducing ro-vibrational transitions for the cyclic three-level system of chiral molecules. Then, at the typical temperature in experiments approximately only the lowest state in the chosen three-level system is thermally occupied and the optical method of enantiomeric-specific state transfer works well. Comparing with the case of purely rotational transitions where all the three states are thermally occupied, this modification will remarkably increase the obtained state-specific enantiomeric enrichment with enantiomeric excess approximately 100%.