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Title: Excitations Partition into Two Distinct Populations in Bulk Perovskites

Abstract

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, 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. 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.

Authors:
 [1];  [2];  [3];  [4];  [1];  [1];  [5];  [6]; ORCiD logo [1]
  1. Department of Chemistry, The James Franck Institute, The Institute for Biophysical Dynamics, The University of Chicago, Chicago IL 60637 USA
  2. The Institute for Molecular Engineering, The University of Chicago, Chicago IL 60637 USA
  3. Materials Science Division, Argonne National Laboratory, Lemont IL 60439 USA
  4. Department of Chemistry, The James Franck Institute, The Institute for Biophysical Dynamics, The University of Chicago, Chicago IL 60637 USA; Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont IL 60439 USA
  5. Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont IL 60439 USA
  6. The Institute for Molecular Engineering, The University of Chicago, Chicago IL 60637 USA; Materials Science Division, Argonne National Laboratory, Lemont IL 60439 USA
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Alfred P. Sloan Foundation; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); U.S. Department of Defense (DOD) - National Security Science and Engineering Faculty Fellowship (NSSEFF)
OSTI Identifier:
1427475
DOE Contract Number:
AC02-06CH11357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Advanced Optical Materials; Journal Volume: 6; Journal Issue: 5
Country of Publication:
United States
Language:
English

Citation Formats

Wang, Lili, Brawand, Nicholas P., Vörös, Márton, Dahlberg, Peter D., Otto, John P., Williams, Nicholas E., Tiede, David M., Galli, Giulia, and Engel, Gregory S. Excitations Partition into Two Distinct Populations in Bulk Perovskites. United States: N. p., 2018. Web. doi:10.1002/adom.201700975.
Wang, Lili, Brawand, Nicholas P., Vörös, Márton, Dahlberg, Peter D., Otto, John P., Williams, Nicholas E., Tiede, David M., Galli, Giulia, & Engel, Gregory S. Excitations Partition into Two Distinct Populations in Bulk Perovskites. United States. doi:10.1002/adom.201700975.
Wang, Lili, Brawand, Nicholas P., Vörös, Márton, Dahlberg, Peter D., Otto, John P., Williams, Nicholas E., Tiede, David M., Galli, Giulia, and Engel, Gregory S. Tue . "Excitations Partition into Two Distinct Populations in Bulk Perovskites". United States. doi:10.1002/adom.201700975.
@article{osti_1427475,
title = {Excitations Partition into Two Distinct Populations in Bulk Perovskites},
author = {Wang, Lili and Brawand, Nicholas P. and Vörös, Márton and Dahlberg, Peter D. and Otto, John P. and Williams, Nicholas E. and Tiede, David M. and Galli, Giulia and Engel, Gregory S.},
abstractNote = {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, 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. 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.},
doi = {10.1002/adom.201700975},
journal = {Advanced Optical Materials},
number = 5,
volume = 6,
place = {United States},
year = {Tue Jan 09 00:00:00 EST 2018},
month = {Tue Jan 09 00:00:00 EST 2018}
}