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Title: Depressed Phase Transitions and Thermally Persistent Local Distortions in CsPbBr3 Quantum Dots

Abstract

The optoelectronic properties of CsPbX3 quantum dots (where X = Cl, Br, or I) are influenced by both their local and average structures. Variable-temperature synchrotron X-ray diffraction measurements of CsPbBr3 quantum dots show that the temperatures for both the orthorhombic-to-tetragonal (50 °C < Tγ-β < 59 °C) and tetragonal-to-cubic (108 °C < Tβ-α < 117 °C) phase transitions of the average structure are depressed relative to their temperatures in bulk CsPbBr3. Simultaneously, pair distribution function (PDF) analysis of syn-chrotron X-ray total scattering measurements indicate that the local crystal structure of the quantum dots is best described as ortho-rhombically distorted over the temperature range of 22 °C < T < 160 °C, with only small changes in the magnitude of the distortion occurring during the observed changes in the average structure. Here, taken together these results suggest that phase transitions in CsPbBr3 quantum dots are order-disorder, involving the gradual ordering of individually coherent domains that cannot be attributed to changes in the surface area or to ferroelectric phenomena.

Authors:
 [1]; ORCiD logo [1]
  1. Univ. of Southern California, Los Angeles, CA (United States)
Publication Date:
Research Org.:
Univ. of Southern California, Los Angeles, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1582648
Grant/Contract Number:  
SC0006812; FG02-11ER4682; AC02-06CH11357; DMR 1720256
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 19; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Cottingham, Patrick, and Brutchey, Richard L. Depressed Phase Transitions and Thermally Persistent Local Distortions in CsPbBr3 Quantum Dots. United States: N. p., 2018. Web. doi:10.1021/acs.chemmater.8b02295.
Cottingham, Patrick, & Brutchey, Richard L. Depressed Phase Transitions and Thermally Persistent Local Distortions in CsPbBr3 Quantum Dots. United States. https://doi.org/10.1021/acs.chemmater.8b02295
Cottingham, Patrick, and Brutchey, Richard L. Sat . "Depressed Phase Transitions and Thermally Persistent Local Distortions in CsPbBr3 Quantum Dots". United States. https://doi.org/10.1021/acs.chemmater.8b02295. https://www.osti.gov/servlets/purl/1582648.
@article{osti_1582648,
title = {Depressed Phase Transitions and Thermally Persistent Local Distortions in CsPbBr3 Quantum Dots},
author = {Cottingham, Patrick and Brutchey, Richard L.},
abstractNote = {The optoelectronic properties of CsPbX3 quantum dots (where X = Cl, Br, or I) are influenced by both their local and average structures. Variable-temperature synchrotron X-ray diffraction measurements of CsPbBr3 quantum dots show that the temperatures for both the orthorhombic-to-tetragonal (50 °C < Tγ-β < 59 °C) and tetragonal-to-cubic (108 °C < Tβ-α < 117 °C) phase transitions of the average structure are depressed relative to their temperatures in bulk CsPbBr3. Simultaneously, pair distribution function (PDF) analysis of syn-chrotron X-ray total scattering measurements indicate that the local crystal structure of the quantum dots is best described as ortho-rhombically distorted over the temperature range of 22 °C < T < 160 °C, with only small changes in the magnitude of the distortion occurring during the observed changes in the average structure. Here, taken together these results suggest that phase transitions in CsPbBr3 quantum dots are order-disorder, involving the gradual ordering of individually coherent domains that cannot be attributed to changes in the surface area or to ferroelectric phenomena.},
doi = {10.1021/acs.chemmater.8b02295},
journal = {Chemistry of Materials},
number = 19,
volume = 30,
place = {United States},
year = {Sat Sep 08 00:00:00 EDT 2018},
month = {Sat Sep 08 00:00:00 EDT 2018}
}

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