Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 7, Issue 4, Pages 715-721Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.5b02888
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Funding
- Office of Basic Energy Sciences of the U.S. Department of Energy [DE-SC0014334]
- Center for Sustainable Energy at Notre Dame (ND Energy)
- King Abdullah University of Science and Technology (KAUST) [OCRF-2014-CRG3-2268]
- Sustainable Energy Initiative (SEI), Center for Sustainable Energy at Notre Dame (ND Energy)
- U.S. Department of Energy (DOE) [DE-SC0014334] Funding Source: U.S. Department of Energy (DOE)
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The facile solution-processability of methyl ammonium lead halide (CH3NH3PbI3) perovskites has catalyzed the development of inexpensive, hybrid perovskite-based optoelectronics. It is apparent, though, that solution processed CH3NH3PbI3 films possess local emission heterogeneities, stemming from electronic disorder in the material. Herein we investigate the spatially resolved emission properties of CH3NH3PbI3 thin films through detailed emission intensity versus excitation intensity measurements. These studies enable us to establish the existence of nonuniform trap density variations wherein regions of CH3NH3PbI3 films exhibit effective free carrier recombination while others exhibit emission dynamics strongly influenced by the presence of trap states. Such trap density variations lead to spatially varying emission quantum yields and correspondingly impact the performance of both methylammonium lead halide perovskite solar cells and other hybrid perovskite-based devices. Of additional note is that the observed spatial extent of the optical disorder extends over length scales greater than that of underlying crystalline domains, suggesting the existence of other factors, beyond grain boundary-related nonradiative recombination channels, which lead to significant intrafilm optical heterogeneities.
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