Chemical Diversity in Lead-Free, Layered Double Perovskites: A Combined Experimental and Computational Approach

Akin to the expansion in compositional diversity that halide double perovskites provided to three-dimensional perovskites, layered double perovskites could further expand the diversity of two-dimensional (2D) perovskites, and therefore, they could also enhance the properties or expand the possible applications of such materials. Despite the great promise of halide 2D double perovskites, up to date, there are only four confirmed members of this family of materials. Herein, we explore 90 hypothetical new members of this family of materials by a combined theoretical, computational, and experimental method. The combination of these tactics allowed us to predict several new materials, out of which we experimentally synthesized and characterized five new layered double perovskites, some of which show promising properties for their use in photovoltaics and optoelectronics. Further, our work highlights the vast diversity of compositions and therefore of applications that double-layered perovskites have yet to offer.