First principle insight into surface/interface engineering for efficient and stable perovskite optoelectronic devices

Recent advancements in perovskite solar cells (PSCs) have significantly improved efficiency, but issues related to stability and charge recombination persist, limiting their long-term performance. Surface/interface engineering has emerged as a critical strategy to address these challenges, enhancing charge transport and reducing recombination near and across interfaces. We explored three different surface/interface treatments from the perspective of density functional theory (DFT) calculations, to improve stability and performance of perovskite solar cells and optoelectronic detectors. These include (i) developing a strong-bonding hole transport layer (HTL) with EtCz3EPA and entinostat, respectively, to strengthen the perovskite-substrate interface, (ii) using P3CT as HTL to suppress deprotonation of PSS in Sb-Pb perovskites, mitigating buried-interface degradation, and (iii) passivating FA vacancies, undercoordinated Pb and Pb-Pb dimers on FAPbBr3 surface using ammonium bromide, facilitating applications in gamma-ray detectors. These strategies offer a pathway to more efficient and stable PSCs and optoelectronic detectors.