Nanoscale heterogeneity of ultrafast many-body carrier dynamics in triple cation perovskites

Jun Nishida, Peter T. S. Chang, Jiselle Y. Ye, Prachi Sharma, Dylan M. Wharton, Samuel C. Johnson, Sean E. Shaheen and Markus B. Raschke ()
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Jun Nishida: University of Colorado
Peter T. S. Chang: University of Colorado
Jiselle Y. Ye: University of Colorado
Prachi Sharma: University of Colorado
Dylan M. Wharton: University of Colorado
Samuel C. Johnson: University of Colorado
Sean E. Shaheen: University of Colorado
Markus B. Raschke: University of Colorado

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract In high fluence applications of lead halide perovskites for light-emitting diodes and lasers, multi-polaron interactions and associated Auger recombination limit the device performance. However, the relationship of the ultrafast and strongly lattice coupled carrier dynamics to nanoscale heterogeneities has remained elusive. Here, in ultrafast visible-pump infrared-probe nano-imaging of the photoinduced carrier dynamics in triple cation perovskite films, a ~20 % variation in sub-ns relaxation dynamics with spatial disorder on tens to hundreds of nanometer is resolved. We attribute the non-uniform relaxation dynamics to the heterogeneous evolution of polaron delocalization and increasing scattering time. The initial high-density excitation results in faster relaxation due to strong many-body interactions, followed by extended carrier lifetimes at lower densities. These results point towards the missing link between the optoelectronic heterogeneity and associated carrier dynamics to guide synthesis and device engineering for improved perovskites device performance.

Date: 2022
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DOI: 10.1038/s41467-022-33935-0

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