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Title: High-Temperature Photoluminescence of CsPbX 3 (X = Cl, Br, I) Nanocrystals

Recent synthetic developments have generated intense interest in the use of cesium lead halide perovskite nanocrystals for light-emitting applications. This work presents the photoluminescence (PL) of cesium lead halide perovskite nanocrystals with tunable halide composition recorded as function of temperature from 80 to 550 K. CsPbBr 3 nanocrystals show the highest resilience to temperature while chloride-containing samples show relatively poorer preservation of photoluminescence at elevated temperatures. Thermal cycling experiments show that PL loss of CsPbBr 3 is largely reversible at temperatures below 450 K, but shows irreversible degradation at higher temperatures. Time-resolved measurements of CsPbX 3 samples show an increase in the PL lifetime with temperature elevation, consistent with exciton fission to form free carriers, followed by a decrease in the apparent PL lifetime due to trapping. In conclusion, PL persistence measurements and time-resolved spectroscopies implicate thermally assisted trapping, most likely to halogen vacancy traps, as the mechanism of reversible PL loss.
Authors:
; ; ;
Publication Date:
Grant/Contract Number:
AC02-06CH11357; 306733
Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 21; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); European Union (EU)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; CsPbX3; high-temperature; perovskites; photoluminescence; stability
OSTI Identifier:
1372060
Alternate Identifier(s):
OSTI ID: 1401060

Diroll, Benjamin T., Nedelcu, Georgian, Kovalenko, Maksym, and Schaller, Richard D.. High-Temperature Photoluminescence of CsPbX3 (X = Cl, Br, I) Nanocrystals. United States: N. p., Web. doi:10.1002/adfm.201606750.
Diroll, Benjamin T., Nedelcu, Georgian, Kovalenko, Maksym, & Schaller, Richard D.. High-Temperature Photoluminescence of CsPbX3 (X = Cl, Br, I) Nanocrystals. United States. doi:10.1002/adfm.201606750.
Diroll, Benjamin T., Nedelcu, Georgian, Kovalenko, Maksym, and Schaller, Richard D.. 2017. "High-Temperature Photoluminescence of CsPbX3 (X = Cl, Br, I) Nanocrystals". United States. doi:10.1002/adfm.201606750. https://www.osti.gov/servlets/purl/1372060.
@article{osti_1372060,
title = {High-Temperature Photoluminescence of CsPbX3 (X = Cl, Br, I) Nanocrystals},
author = {Diroll, Benjamin T. and Nedelcu, Georgian and Kovalenko, Maksym and Schaller, Richard D.},
abstractNote = {Recent synthetic developments have generated intense interest in the use of cesium lead halide perovskite nanocrystals for light-emitting applications. This work presents the photoluminescence (PL) of cesium lead halide perovskite nanocrystals with tunable halide composition recorded as function of temperature from 80 to 550 K. CsPbBr3 nanocrystals show the highest resilience to temperature while chloride-containing samples show relatively poorer preservation of photoluminescence at elevated temperatures. Thermal cycling experiments show that PL loss of CsPbBr3 is largely reversible at temperatures below 450 K, but shows irreversible degradation at higher temperatures. Time-resolved measurements of CsPbX3 samples show an increase in the PL lifetime with temperature elevation, consistent with exciton fission to form free carriers, followed by a decrease in the apparent PL lifetime due to trapping. In conclusion, PL persistence measurements and time-resolved spectroscopies implicate thermally assisted trapping, most likely to halogen vacancy traps, as the mechanism of reversible PL loss.},
doi = {10.1002/adfm.201606750},
journal = {Advanced Functional Materials},
number = 21,
volume = 27,
place = {United States},
year = {2017},
month = {3}
}

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