Interfacial engineering dominated passivation strategy to facilitate performance improvement of CsSnCl3 PSCs by induced Sn–O bonds: Insight from DFT calculations and device simulations

Defect passivation of perovskite surface not only reduces non-radiative recombination due to defect trapping charge, but also modulates the interfacial structure and energy levels, making it an effective means of solving the stability problem of perovskite materials. This work provides a passivation strategy for CsSnCl3 perovskite, and the interfacial interactions between CsSnCl3 and the passivation agent (PbSO4 and PbCO3) are explored based on first-principles density functional theory. By introducing PbSO4 and PbCO3 with multifunctional quantum dots, strong Sn-O bonds are formed with unsaturated coordination and dangling bonds on the surface of CsSnCl3. Binding sites of water molecules and impurities would be occupied by these bonds, to achieve surface passivation and dehumidification effects, and significantly improve the optical properties of CsSnCl3. PbCO3/SnCl and PbSO4/SnCl constructed the satisfactory interfacial energy level structures. PbCO3/SnCl exhibited excellent light absorption performance ranging in 0 ∼ 1200 nm. Introducing PbSO4 and PbCO3 reduced the refractive index of CsSnCl3 exhibiting excellent extinction properties. According to the simulation of Solar Design, perovskite solar cells (PSCs) constructed by (PbSO4, PbCO3)/CsSnCl3 as the active layer achieved power conversion efficiencies of 15.1946 % and 17.3783 %, respectively. This work's research and design results provide a passivation strategy and PSCs design scheme for CsSnCl3 surface defects, which is of great significance for further modification of CsSnCl3 to better apply in photovoltaic field.