Climbing the rotational ladder to chirality

Abstract: Molecular chirality is conventionally understood as space-inversion-symmetry breaking in the equilibrium structure of molecules. Less well known is that achiral molecules can be made chiral through extreme rotational excitation. Here, we theoretically demonstrate a clear strategy for generating rotationally-induced chirality (RIC): An optical centrifuge rotationally excites the phosphine molecule (PH$_3$) into chiral cluster states that correspond to clockwise ($R$-enantiomer) or anticlockwise ($L$-enantiomer) rotation about axes almost coinciding with single P-H bonds. Application of a strong dc electric field during the centrifuge pulse favors the production of one rotating enantiomeric form over the other, creating dynamically chiral molecules with $permanently$ oriented rotational angular momentum. This essential step toward characterizing RIC promises a fresh perspective on chirality as a fundamental aspect of nature.