Vapor-assisted deposition of highly efficient, stable black-phase FAPbI perovskite solar cells.

Mixtures of cations or halides with FAPbI (where FA is formamidinium) lead to high efficiency in perovskite solar cells (PSCs) but also to blue-shifted absorption and long-term stability issues caused by loss of volatile methylammonium (MA) and phase segregation. We report a deposition method using MA thiocyanate (MASCN) or FASCN vapor treatment to convert yellow δ-FAPbI perovskite films to the desired pure α-phase. NMR quantifies MA incorporation into the framework. Molecular dynamics simulations show that SCN anions promote the formation and stabilization of α-FAPbI below the thermodynamic phase-transition temperature. We used these low-defect-density α-FAPbI films to make PSCs with >23% power-conversion efficiency and long-term operational and thermal stability, as well as a low (330 millivolts) open-circuit voltage loss and a low (0.75 volt) turn-on voltage of electroluminescence.