Excitations Partition into Two Distinct Populations in Bulk Perovskites

Wang, Lili; Brawand, Nicholas P.; Voros, Marton; Dahlberg, Peter D.; Otto, John P.; Williams, Nicholas E.; Tiede, David M.; Galli, Giulia; Engel, Gregory S.

doi:10.1002/adom.201700975

Excitations Partition into Two Distinct Populations in Bulk Perovskites

Journal Article · Tue Jan 09 00:00:00 UTC 2018 · Advanced Optical Materials

DOI:https://doi.org/10.1002/adom.201700975· OSTI ID:1427475

Wang, Lili ^[1]; Brawand, Nicholas P. ^[2]; Voros, Marton ^[3]; Dahlberg, Peter D. ^[1]; Otto, John P. ^[1]; Williams, Nicholas E. ^[1]; Tiede, David M. ^[4]; Galli, Giulia ^[5]; ^[1]

Univ. of Chicago, IL (United States). James Franck Inst., and Inst. for Biophysical Dynamics
Univ. of Chicago, IL (United States). Inst. for Molecular Engineering
Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Argonne National Lab. (ANL), Argonne, IL (United States).Chemical Sciences and Engineering Division
Univ. of Chicago, IL (United States). Inst. for Molecular Engineering; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division

Organolead halide perovskites convert optical excitations to charge carriers with remarkable efficiency in optoelectronic devices. Previous research predominantly documents dynamics in perovskite thin films; however, extensive disorder in this platform may obscure the observed carrier dynamics. Here in this study, carrier dynamics in perovskite single-domain single crystals is examined by performing transient absorption spectroscopy in a transmissive geometry. Two distinct sets of carrier populations that coexist at the same radiation fluence, but display different decay dynamics, are observed: one dominated by second-order recombination and the other by third-order recombination. Based on ab initio simulations, this observation is found to be most consistent with the hypothesis that free carriers and localized carriers coexist due to polaron formation. Lastly, the calculations suggest that polarons will form in both CH₃NH₃PbBr₃ and CH₃NH₃PbI₃ crystals, but that they are more pronounced in CH₃NH₃PbBr₃. Single-crystal CH₃NH₃PbBr₃ could represent the key to understanding the impact of polarons on the transport properties of perovskite optoelectronic devices.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Alfred P. Sloan Foundation; National Science Foundation (NSF); U.S. Department of Defense (DOD). National Security Science and Engineering Faculty Fellowship (NSSEFF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1427475

Alternate ID(s):: OSTI ID: 1416406
OSTI ID: 1433053

Journal Information:: Advanced Optical Materials, Journal Name: Advanced Optical Materials Journal Issue: 5 Vol. 6; ISSN 2195-1071

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Structural fluctuations cause spin-split states in tetragonal (CH ₃ NH ₃ )PbI ₃ as evidenced by the circular photogalvanic effect Niesner, Daniel; Hauck, Martin; Shrestha, Shreetu Proceedings of the National Academy of Sciences, Vol. 115, Issue 38 https://doi.org/10.1073/pnas.1805422115	journal	September 2018