Abstract
This work derived the relationship between the concentrations of Pb(2+) and I(-) vacancies, along with MA(+) vacancies, in MAPbI(3) crystals and their effect on the short-circuit current of MAPbI(3)-based solar photovoltaic devices. First principles calculations revealed that Pb(2+) and I(-) vacancies introduce shallow defect levels near the Fermi level, acting as non-radiative recombination centers, which significantly influence the short-circuit current and open-circuit voltage. In contrast, MA(+) vacancies have a negligible effect on the optoelectronic properties of MAPbI(3). Based on this correlation, we successfully elucidated the declining trend of the short-circuit current (J(sc)) in MAPbI(3)-based devices with increasing Pb(2+)/I(-) vacancy concentrations, while uncovering the microscopic mechanism responsible for the minor performance impact of MA(+) vacancies.