Elimination of Charge Recombination Centers in Metal Halide Perovskites by Strain.

Metal halide perovskites exhibit enhanced photoluminescence and long-lived carriers in experiments under strain. Using ab initio nonadiabatic molecular dynamics, we demonstrate that compressive and tensile strain can eliminate charge recombination centers created by defect states, by shifting traps from bandgap into bands. A compressive strain enhances coupling of Pb-s and I-p orbitals, pushes the valence band (VB) up in energy, and moves the trap state due to iodine interstitial (Ii) into the VB. The strain distorts the system and breaks the I-dimer responsible for the Ii trap. A tensile strain increases Pb-Pb distance, weakens overlap of Pb-p orbitals, and pushes the conduction band (CB) down in energy. The trap state created by replacement of iodine with methylammonium (MAI) is moved into the CB. Application of strain to the defective systems not only eliminates midgap traps but also creates moderate disorder that reduces overlap of electron and hole wave functions, activates phonon modes accelerating coherence loss within the electronic subsystem, and extends carrier lifetimes even beyond those in pristine MAPbI3. Our investigation rationalizes the high performance of perovskites solar cells under strain and reveals how strain passivates Ii and MAI defects in MAPbI3, providing a new nonchemical strategy for defect control and engineering.