High-Temperature Photoluminescence of CsPbX3 (X = Cl, Br, I) Nanocrystals

Benjamin T. Diroll; Georgian Nedelcu; Maksym V. Kovalenko; Richard D. Schaller

doi:10.1002/adfm.201606750

High-Temperature Photoluminescence of CsPbX₃ (X = Cl, Br, I) Nanocrystals

Benjamin T. Diroll, Georgian Nedelcu, Maksym V. Kovalenko, Richard D. Schaller^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

273 Scopus citations

Abstract

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. PL persistence measurements and time-resolved spectroscopies implicate thermally assisted trapping, most likely to halogen vacancy traps, as the mechanism of reversible PL loss.

Original language	English (US)
Article number	1606750
Journal	Advanced Functional Materials
Volume	27
Issue number	21
DOIs	https://doi.org/10.1002/adfm.201606750
State	Published - Jun 6 2017

Funding

Use of the Center for Nanoscale Materials, an Office of Science user facility, was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Contract No. DE-AC02-06CH11357. M.V.K. acknowledges financial support from the European Union through the FP7 (ERC Starting Grant NANOSOLID, GA No. 306733).

Keywords

CsPbX
high-temperature
perovskites
photoluminescence
stability

ASJC Scopus subject areas

General Chemistry
General Materials Science
Condensed Matter Physics

Access to Document

10.1002/adfm.201606750

Cite this

@article{1252f0cb71a0401caecde04b1b42f98a,

title = "High-Temperature Photoluminescence of CsPbX3 (X = Cl, Br, I) Nanocrystals",

abstract = "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. PL persistence measurements and time-resolved spectroscopies implicate thermally assisted trapping, most likely to halogen vacancy traps, as the mechanism of reversible PL loss.",

keywords = "CsPbX, high-temperature, perovskites, photoluminescence, stability",

author = "Diroll, {Benjamin T.} and Georgian Nedelcu and Kovalenko, {Maksym V.} and Schaller, {Richard D.}",

note = "Publisher Copyright: {\textcopyright} 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2017",

month = jun,

day = "6",

doi = "10.1002/adfm.201606750",

language = "English (US)",

volume = "27",

journal = "Advanced Functional Materials",

issn = "1616-301X",

publisher = "Wiley-VCH Verlag",

number = "21",

}

TY - JOUR

T1 - High-Temperature Photoluminescence of CsPbX3 (X = Cl, Br, I) Nanocrystals

AU - Diroll, Benjamin T.

AU - Nedelcu, Georgian

AU - Kovalenko, Maksym V.

AU - Schaller, Richard D.

PY - 2017/6/6

Y1 - 2017/6/6

N2 - 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. PL persistence measurements and time-resolved spectroscopies implicate thermally assisted trapping, most likely to halogen vacancy traps, as the mechanism of reversible PL loss.

AB - 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. PL persistence measurements and time-resolved spectroscopies implicate thermally assisted trapping, most likely to halogen vacancy traps, as the mechanism of reversible PL loss.

KW - CsPbX

KW - high-temperature

KW - perovskites

KW - photoluminescence

KW - stability

UR - http://www.scopus.com/inward/record.url?scp=85016785154&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85016785154&partnerID=8YFLogxK

U2 - 10.1002/adfm.201606750

DO - 10.1002/adfm.201606750

M3 - Article

AN - SCOPUS:85016785154

SN - 1616-301X

VL - 27

JO - Advanced Functional Materials

JF - Advanced Functional Materials

IS - 21

M1 - 1606750

ER -