Improved Defect Tolerance and Charge Carrier Lifetime in Tin–Lead Mixed Perovskites: Ab Initio Quantum Dynamics

Simulations by nonadiabatic (NA) molecular dynamics demonstrate that mixing tin with lead in CH₃NH₃PbI₃ can passivate the midgap state created by an interstitial iodine (I_i) via the imposed compressive strain and upshifted valence band maximum, reduce NA coupling by decreasing electron-hole wave functions overlap, and shortens pure-dephasing time by introducing high-frequency phonon modes. Thus, the charge carrier lifetime extends to 3.6 ns due to the significantly reduced nonradiative electron-hole recombination, which is an order of magnitude longer than the I_i-containing CH₃NH₃PbI₃, over 2.5 times longer than the pristine CH₃NH₃PbI₃ (1.4 ns), and even 1.7 times longer than the tin-lead mixed perovskite without the I_i defects (2.1 ns). Tin-lead alloying simultaneously increases the I_i defect formation energy to 0.402 eV from 0.179 eV in CH₃NH₃PbI₃, which effectively enhances defect tolerance by reducing the defect concentration. The study reveals the factors controlling the enhanced performance of tin-lead mixed perovskite solar cells.