Piezogyration and elastogyration in ternary chalcopyrites from first principles

Abstract

Natural optical activity arises from the spatial dispersion of the optical response and is described by the rank-two gyration pseudotensor. Its dependence on mechanical stress and strain, quantified by the piezogyration and elastogyration tensors, respectively, has been investigated experimentally for decades. However, a systematic first-principles description of these effects remains largely unexplored. Here we present a first-principles methodology to compute the full piezogyration and elastogyration tensors, and apply it to a set of representative ternary chalcopyrite crystals. The gyration of the unstrained crystal turns out to be a poor predictor of the magnitude of the elastogyration response, which we find to be a property inherited from their parent zinc-blende structures. The elastic compliance tensor further shapes the piezogyration response, with particularly pronounced effects in AgGaS$_2$, a well-known achiral yet optically active crystal. Finally, we explore strain-induced chirality through the trace of the gyration tensor, the only pseudoscalar contribution to the natural optical activity that is linear in the tensor components and encodes information about chirality.