基于环状三能级系统的对映体特异性振转态转移中热布居数影响的消除
Evading thermal population influence in enantiomeric-specific state transfer based on a cyclic three-level system via ro-vibrational transitions
摘要：
基于手性分子的环状三能级体系，从理论上提出了对映体特异性态转移的光学方法。根据这些理论方法，近年来在实验上取得了突破性进展[S. Eibenberger等人，物理修订版信函118，123002（2017）; C. Pérez等人，Angew. Chem.Int.Ed.56，12512（2017）]，但具有低的状态特异性对映体富集。其中一个限制因素是实验中所选的三个纯转动态的热布居数的影响。在这里，我们从理论上提出了一种改进的光学方法的对映体特定的状态转移，有效地避免这样的不利影响的热布居通过引入振转跃迁的环状三能级系统的手性分子。然后，在实验中的典型温度下，近似地只有所选三能级系统中的最低态被热占据，并且光学方法的对映体特异性态转移工作良好。与纯转动跃迁的情况下，所有的三个状态是热占领，这种修改将显着增加所获得的特定状态的对映体富集与对映体过量约100%。
英文摘要：
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%.
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