Excitations Partition into Two Distinct Populations in Bulk Perovskites

Wang, Lili; Brawand, Nicholas P.; Vörös, Márton; 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 04:00:00 UTC 2018 · Advanced Optical Materials

DOI:https://doi.org/10.1002/adom.201700975· OSTI ID:1433053

Wang, Lili ^[1]; Brawand, Nicholas P. ^[2]; Vörös, Márton ^[3]; Dahlberg, Peter D. ^[4]; Otto, John P. ^[1]; Williams, Nicholas E. ^[1]; Tiede, David M. ^[5]; Galli, Giulia ^[6]; ^[1]

Department of Chemistry, The James Franck Institute, The Institute for Biophysical Dynamics, The University of Chicago, Chicago IL 60637 USA
The Institute for Molecular Engineering, The University of Chicago, Chicago IL 60637 USA
Materials Science Division, Argonne National Laboratory, Lemont IL 60439 USA
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
Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont IL 60439 USA
The Institute for Molecular Engineering, The University of Chicago, Chicago IL 60637 USA; Materials Science Division, Argonne National Laboratory, Lemont IL 60439 USA

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.

Research Organization:: Argonne National Laboratory (ANL)

Sponsoring Organization:: Air Force Research Laboratory (AFRL) - Air Force Office of Scientific Research (AFOSR); University of Chicago - Materials Research Science & Engineering Center (MRSEC); Alfred P. Sloan Foundation; USDOE Office of Science - Office of Basic Energy Sciences - Materials Sciences and Engineering Division - Midwest Integrated Center for Computational Materials (MICCoM)

DOE Contract Number:: AC02-06CH11357

OSTI ID:: 1433053

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

Publisher:: Wiley

Country of Publication:: United States

Language:: English

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