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HighlightsDevice simulations and first-principle calculations are employed to derive a guideline for the optimization of CsPbI 3 -based perovskite solar cells (PSCs).    The open voltage and power conversion efficiency of the PSCs are, respectively, improved to 1.31 V and 21.06% by simultaneously introducing an ultra-thin TiO 2  buffer layer and increasing the doping concentration of the ZnO electron transport layer.    The influence of the interfacial buffer layer and doping of the CsPbI 3 /ZnO interface on PSC performance is discussed.Electronic supplementary material  The online version of this article (10.1007/s40820-019-0320-y) contains supplementary material, which is available to authorized users.

Optimizing the Performance of CsPbI3-Based Perovskite Solar Cells via Doping a ZnO Electron Transport Layer Coupled with Interface Engineering