Theoretical Study to Improve Stability and Efficiency for Tin-based Halide Perovskites
Ki-Ha Hong a
a Hanbat National University, 125 Dongseo-daero, Yuseong-gu, Daejeon-si, Korea, Republic of
Materials for Sustainable Development Conference (MATSUS)
Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
#PbFreePero - The potential of lead-free perovskites: synthesis, properties, and applications
Barcelona, Spain, 2022 October 24th - 28th
Organizers: Loreta Muscarella, Eline Hutter and Hendrik Bolink
Poster, Ki-Ha Hong, 292
Publication date: 11th July 2022

Metal halide perovskites (MHPs) have attracted tremendous interest in the fields of solar cells and light-emitting devices thanks to prominent intrinsic properties like defect robustness and good synthesizability. Despite various advantages of MHPs, toxicity is a major concern for their commercialization because archetypical MHPs contain Lead (Pb). There have been tremendous efforts to find alternatives to Pb-based perovskites using computational and experimental methods. However, the certified efficiency of Pb-free candidates is still far behind that of Pb-analogs. Sn-based perovskites have shown the best performance among Pb-free candidates. However, the stability of Sn-based perovskites is worse than Pb-based solar cells. Various combination of A-site cation molecules has been tested to enhance the efficiency and the stability of Sn-based perovskite solar cells. Although Cesium has better potential than other molecular cations in terms of chemical and thermal stability, the performance of Cs-based solar cells is inferior to that of molecular cation-based photovoltaic cells. This study presents various engineering methods to enhance the stability and efficiency of Cs-based tin perovskites solar cells using theoretical methods. We have explored the role of SnX2 (X=F, Cl, Br) additives and alkali metal interstitials on the stability of CsSnI3 films and devices using density functional theory calculations. Our comparative study for various candidate compositions revealed that SnBr2 and K show the most promising behavior among considered additives and interstitials, respectively, regarding stability and efficiency. In addition, dual-site compositional engineering on A- and X- sites are investigated with ab initio thermodynamics. The best composition having optimum bandgap and phase stability is explored by comparing the formation energies of yellow and black phases.

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