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Layered Halide Double Perovskites Cs3+nM(II)nSb2X9+3n (M = Sn, Ge) for Photovoltaic Applications.

Over the past few years, the development of lead-free and stable perovskite absorbers with excellent performance has attracted extensive attention. Much effort has been devoted to screening and synthesizing this type of solar cell absorbers. Here, we present a general design strategy for designing the layered halide double perovskites Cs3+nM(II)nSb2X9+3n (M = Sn, Ge) with desired photovoltaic-relevant properties by inserting [MX6] octahedral layers, based on the principles of increased electronic dimensionality. Compared to Cs3Sb2I9, more suitable band gaps, smaller carrier effective masses, larger dielectric constants, lower exciton binding energies, and higher optical absorption can be achieved by inserting variable [SnI6] or [GeI6] octahedral layers into the [Sb2I9] bilayers. Moreover, our results show that adjusting the thickness of inserted octahedral layers is an effective approach to tune the band gaps and carrier effective masses in a large range. Our work provides useful guidance for designing the promising layered antimony halide double perovskite absorbers for photovoltaic applications.