Coherent Enantiomer‐Selective Population Enrichment Using Tailored Microwave Fields

We report the experimental demonstration of coherent enantiomer‐selective enrichment of chiral molecules by employing a novel microwave five‐pulse scheme. Our results show that enantiomers can be selectively transferred to a rotational level of choice by applying sequences of resonant microwave pulses in a phase‐ and polarization‐controlled manner. This is achieved by simultaneously exciting all three kinds of electric dipole‐allowed rotational transitions and monitoring the effect on a fourth rotational transition of choice. Using molecular beams, we apply our method to two chiral terpenes and obtain a 6 % enantiomeric enrichment, which is one order of magnitude larger than that recently reported in a buffer‐gas cell experiment. This approach establishes a robust scheme for controlled manipulation of enantiomers using tailored microwave fields and opens up new avenues for chiral purification and enrichment that can be used in a broad scope of analytical or spectroscopic applications.