Rational pulse design for enantiomer-selective microwave three-wave mixing

Abstract

Microwave three-wave mixing allows for enantiomer-selective excitation of randomly oriented chiral molecules into rotational states with different energy. The random orientation of molecules is reflected in the degeneracy of the rotational spectrum with respect to the orientational quantum number $M$ and reduces, if not accounted for, enantiomer-selectivity. Here, we show how to design pulse sequences with maximal enantiomer-selectivity from an analysis of the $M$-dependence of the Rabi frequencies associated with rotational transitions induced by resonant microwave drives. We compare different excitations schemes for rotational transitions and show that maximal enantiomer-selectivity at a given rotational temperature is achieved for synchronized three-wave mixing with circularly polarized fields.

The arXiv publication contains corrected Figures 5(c) and 6(c). The editors of Symmetry did not allow us to publish an erratum, despite the relevance of the correction to anyone who would want to utilize these pulses. The error consists in the wrong labeling of the pulses. The pulse sequence as shown in Symmetry 14, 871 (2022) would not result in enantioselectivity

References in corpus (4)

• Enantiomer-Specific State Transfer of Chiral Molecules
• Controlled enantioselective orientation of chiral molecules with an optical centrifuge
• Principles of enantio-selective excitation in three-wave mixing spectroscopy of chiral molecules
• State-specific Enrichment of Chiral Conformers with Microwave Spectroscopy