Enantioselective Topological Frequency Conversion

Abstract

Two molecules are enantiomers if they are non-superimposable mirror images of each other. Electric dipole-allowed cyclic transitions $|1\rangle\to|2\rangle\to|3\rangle\to|1\rangle$ obey the symmetry relation $\mathcal{O}^{R}=-\mathcal{O}^{S}$, where $\mathcal{O}^{R,S}=(\mu_{21}^{R,S}E_{21})(\mu_{13}^{R,S}E_{13})(\mu_{32}^{R,S}E_{32})$, and $R,S$ label the two enantiomers. Here we generalize the concept of topological frequency conversion to an ensemble of enantiomers. We show that, within a rotating-frame, the pumping power between fields of frequency $\omega_{1}$ and $\omega_{2}$ is sensitive to enantiomeric excess, $\mathcal{P}_{2\to1}=\hbar\frac{\omega_{1}\omega_{2}C_{L}^{R}}{2\pi}(N_{R}-N_{S})$, where $N_{i}$ is the number of enantiomers $i$ and $C_{L}^{R}$ is an enantiomer-dependent Chern number. Connections with chiroptical microwave spectroscopy are made. Our work provides an underexplored and fertile connection between topological physics and molecular chirality.