Temperature and Gate Dependence of Carrier Diffusion in Single Crystal Methylammonium Lead Iodide Perovskite...

We investigate temperature-dependent photogenerated carrier diffusion in single-crystal methylammonium lead iodide microstuctures via scanning photocurrent microscopy. Carrier diffusion lengths increased abruptly across the tetragonal to orthorhombic phase transition and reached 200 ± 50 μm at 80 K. In combination with the microsecond carrier lifetime measured by a transient photocurrent method, an enormous carrier mobility value of 3 × 10⁴ cm²/V s was extracted at 80 K. The observed highly nonlocal photocurrent and the rapid increase of the carrier diffusion length at low temperatures can be understood by the formation and efficient transport of free excitons in the orthorhombic phase as a result of reduced optical phonon scattering due to the dipolar nature of the excitons. Carrier diffusion lengths were tuned by a factor of 8 by gate voltage and increased with increasing majority carrier (electron) concentration, consistent with the exciton model.