Materials Discovery of Stable and Nontoxic Halide Perovskite Materials for High‐Efficiency Solar Cells

Abstract

Two critical limitations of organic-inorganic lead halide perovskite materials for solar cells are their poor stability in humid environments and inclusion of toxic lead. In this study, high-throughput density functional theory (DFT) methods are used to computationally model and screen 1845 halide perovskites in search of new materials without these limitations that are promising for solar cell applications. This study focuses on finding materials that are comprised of nontoxic elements, stable in a humid operating environment, and have an optimal bandgap for one of single junction, tandem Si-perovskite, or quantum dot-based solar cells. Single junction materials are also screened on predicted single junction photovoltaic (PV) efficiencies exceeding 22.7%, which is the current highest reported PV efficiency for halide perovskites. Generally, these methods qualitatively reproduce the properties of known promising nontoxic halide perovskites that are either experimentally evaluated or predicted from theory. From a set of 1845 materials, 15 materials pass all screening criteria for single junction cell applications, 13 of which are not previously investigated, such as (CH 3 NH 3 ) 0.75 Cs 0.25 SnI 3 , ((NH 2 ) 2 CH) Ag 0.5 Sb 0.5 Br 3 , CsMn 0.875 Fe 0.125 I 3 , ((CH 3 ) 2 NH 2 )Ag 0.5 Bi 0.5 I 3 , and ((NH 2 ) 2 CH) 0.5 Rb 0.5 SnI 3 . These materials, together with others predicted in this study, may be promising candidate materials for stable, highly efficient, and nontoxic perovskite-based solar cells.

Bayesian optimization based on a unified figure of merit for accelerated materials screening: A case study of halide perovskites

“…4), and electronic structure (Nos. [5][6][7][8][9][10][11][12][13][14]. Use of all fourteen features may lead to a waste of resources and over-fitting.…”

“…According to calculations by Jacobs et al [10], the optimal range for the PBE-calculated bandgap is within 0.6-1.2 eV, with the optimal value being around 0.9 eV. Therefore, we established the formula as the objective Table 2.…”

“…Design of novel materials in the fields of catalysis [1][2][3] and photovoltaics [4][5][6][7][8][9][10] is highly dependent on the figure of merit, which relates material functionality to material parameters. For a long time, the bandgap (E g ) has been considered as a crucial material parameter in the search of novel semiconductors for photovoltaic applications subject to the Shockely-Queisser limit [11].…”

“…Huo et al [9] used high-throughput computing based on phase stability, formation energy, bandgap, effective mass, and optical absorption to select five compounds among 168 types of chalcogenide single perovskites. Jacobs et al [10] sequentially considered energy above the convex hull, the Perdew-Burke-Ernzerhof (PBE)-bandgap, the Heyd-Scuseria-Ernzerhof (HSE)-bandgap, and spectroscopic limited maximum efficiency (SLME) calculations, and finally selected 15 perovskites for potential solar cell applications.…”

Exotic Structural and Optoelectronic Properties of Layered Halide Double Perovskite Polymorphs

“…[ 39–41 ] For example, though α‐CsPbI 3 , MAPbI 3 , and MASnI 3 were calculated to be unstable with higher energy than its decomposed constituents, they can still be synthesized in experiments. [ 42 ]…”