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Title: Pressure-Induced Phase Changes in Cesium Lead Bromide Perovskite Nanocrystals with and without Ruddlesden–Popper Faults

Abstract

Lead halide perovskites have a rich landscape of structural and optical properties, which can be explored and possibly controlled by applying high pressure. In contrast to several reports on high pressure studies of CsPbBr 3 nanocrystals (NCs), there have so far been no studies under pressure that incorporate planar defects. CsPbBr 3 NCs with Ruddlesden-Popper faults (RP), formed via post-synthetic fusion growth, are significantly larger in size than as-synthesized NCs and display exceptional emission stability. Here, we compare synchrotron-based high pressure X-ray diffraction and photoluminescence (PL) properties of CsPbBr3 (without RP) and RP-CsPbBr 3 (with RP), and resolve their crystal structure under pressure for the first time. CsPbBr3 undergoes a phase transition from orthorhombic Pnma phase at ambient pressure to cubic Pm$$\bar{3}$$m phase at 1.7 GPa and RP-CsPbBr 3 transforms from Pnma to the monoclinic P2 1/m phase at 0.74 GPa in addition to several isostructural transitions. Density-functional calculations predict a narrowing of the band gap with pressure, concomitant with the PL energies. The RP-CsPbBr 3 NCs exhibit enhanced PL intensity at 1 GPa and show band gap opening at high pressures. Our work opens new strategies for tuning not just the structural properties but also tuning planar defects in alkali halide lead crystals for improved optical properties.

Authors:
 [1];  [1];  [1];  [1];  [2]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Missouri, Columbia, MO (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Univ. of Missouri, Columbia, MO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1595474
Grant/Contract Number:  
SC0019109; DMR-1807263; DMR-1810922; AC02-06CH11357
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 32; Journal Issue: 2; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Yesudhas, Sorb, Morrell, Maria V., Anderson, Matthew J., Ullrich, Carsten A., Kenney-Benson, Curtis, Xing, Yangchuan, and Guha, Suchismita. Pressure-Induced Phase Changes in Cesium Lead Bromide Perovskite Nanocrystals with and without Ruddlesden–Popper Faults. United States: N. p., 2019. Web. doi:10.1021/acs.chemmater.9b04157.
Yesudhas, Sorb, Morrell, Maria V., Anderson, Matthew J., Ullrich, Carsten A., Kenney-Benson, Curtis, Xing, Yangchuan, & Guha, Suchismita. Pressure-Induced Phase Changes in Cesium Lead Bromide Perovskite Nanocrystals with and without Ruddlesden–Popper Faults. United States. doi:10.1021/acs.chemmater.9b04157.
Yesudhas, Sorb, Morrell, Maria V., Anderson, Matthew J., Ullrich, Carsten A., Kenney-Benson, Curtis, Xing, Yangchuan, and Guha, Suchismita. Thu . "Pressure-Induced Phase Changes in Cesium Lead Bromide Perovskite Nanocrystals with and without Ruddlesden–Popper Faults". United States. doi:10.1021/acs.chemmater.9b04157.
@article{osti_1595474,
title = {Pressure-Induced Phase Changes in Cesium Lead Bromide Perovskite Nanocrystals with and without Ruddlesden–Popper Faults},
author = {Yesudhas, Sorb and Morrell, Maria V. and Anderson, Matthew J. and Ullrich, Carsten A. and Kenney-Benson, Curtis and Xing, Yangchuan and Guha, Suchismita},
abstractNote = {Lead halide perovskites have a rich landscape of structural and optical properties, which can be explored and possibly controlled by applying high pressure. In contrast to several reports on high pressure studies of CsPbBr3 nanocrystals (NCs), there have so far been no studies under pressure that incorporate planar defects. CsPbBr3 NCs with Ruddlesden-Popper faults (RP), formed via post-synthetic fusion growth, are significantly larger in size than as-synthesized NCs and display exceptional emission stability. Here, we compare synchrotron-based high pressure X-ray diffraction and photoluminescence (PL) properties of CsPbBr3 (without RP) and RP-CsPbBr3 (with RP), and resolve their crystal structure under pressure for the first time. CsPbBr3 undergoes a phase transition from orthorhombic Pnma phase at ambient pressure to cubic Pm$\bar{3}$m phase at 1.7 GPa and RP-CsPbBr3 transforms from Pnma to the monoclinic P21/m phase at 0.74 GPa in addition to several isostructural transitions. Density-functional calculations predict a narrowing of the band gap with pressure, concomitant with the PL energies. The RP-CsPbBr3 NCs exhibit enhanced PL intensity at 1 GPa and show band gap opening at high pressures. Our work opens new strategies for tuning not just the structural properties but also tuning planar defects in alkali halide lead crystals for improved optical properties.},
doi = {10.1021/acs.chemmater.9b04157},
journal = {Chemistry of Materials},
issn = {0897-4756},
number = 2,
volume = 32,
place = {United States},
year = {2019},
month = {12}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on December 26, 2020
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