Organic Molecular Dynamics and Charge-carrier Lifetime in Lead Iodide Perovskite MAPbI$_3$

The long charge carrier lifetime of the hybrid organic-inorganic perovskites (HOIPs) is the key for their remarkable performance as a solar cell material. The microscopic mechanism for the long lifetime is still in debate. Here, by using muon spin relaxation technique that probes the fluctuation of local magnetic fields, we show that the muon depolarization rate ($Δ$) of a prototype HOIP methylammonium lead iodide (MAPbI$_3$) shows a sharp decrease with increasing temperature in two steps above 120 K and 190 K across the structural transition from orthorhombic to tetragonal structure at 162 K. Our analysis shows that the reduction of $Δ$ is quantitatively in agreement with the expected behavior due to the rapid development of MA jumping rotation around the $C_3$ and $C_4$ symmetry axes. Our results provide direct evidence for the intimate relation between the rotation of the electric dipoles of MA molecules and the charge carrier lifetime in HOIPs.

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