Evolutionary search for BiInS3 crystal structure and predicting its second-order nonlinear optical property

We used ab initio evolutionary algorithm to predict the stable and energetically competitive metastable structures of the nonlinear optical materials BiInS3 crystal. The powerful evolutionary algorithm allows us to find the global minimum of the energy landscape with dramatic reduced candidate numbers. Combining geometry optimization with density functional method and the phonon dispersion calculation it is possible for us to determine the stable structure of BiInS3 within only several tens of thousand candidates. The proposed most stable structure adopts the P21 space group, and its second-harmonic generation coefficient is as large as 59 pm/v. The former synthesized BiInS3 is probable corresponding to the metastable Pnma structure. The existence of iso-energy structures at the metastable energy range suggests that more delicate synthetic method is required to obtain high quality BiInS3 crystal.

The most stable P21 structure (left) and the meta-stable Pnma structure (right) for BiInS3 crystal predicted by ab initio evolutionary algorithm.Figure optionsDownload as PowerPoint slideHighlights
► BiInS3 crystal structure was predicted by evolutionary algorithm.
► Electronic structure of BiInS3 was studied by density functional theory.
► Nonlinear optical property was calculated for BiInS3.
► BiInS3 has large second-harmonic generation coefficient in mid-infrared region.