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

Journal Article · · Chemistry of Materials
 [1];  [2];  [2];  [2];  [3]; ORCiD logo [2]; ORCiD logo [2]
  1. Univ. of Missouri, Columbia, MO (United States); University of Missouri
  2. Univ. of Missouri, Columbia, MO (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
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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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Univ. of Missouri, Columbia, MO (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC)
Grant/Contract Number:
AC02-06CH11357; SC0019109
OSTI ID:
1595474
Journal Information:
Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 2 Vol. 32; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (47)

Temperature Dependent Photoluminescence of MBE Grown Gallium Nitride Quantum Dots journal November 2001
Low-Temperature Absorption, Photoluminescence, and Lifetime of CsPbX 3 (X = Cl, Br, I) Nanocrystals journal May 2018
50-Fold EQE Improvement up to 6.27% of Solution-Processed All-Inorganic Perovskite CsPbBr 3 QLEDs via Surface Ligand Density Control journal November 2016
Nanocube Superlattices of Cesium Lead Bromide Perovskites and Pressure-Induced Phase Transformations at Atomic and Mesoscale Levels journal March 2017
Stable Light-Emitting Diodes Using Phase-Pure Ruddlesden-Popper Layered Perovskites journal January 2018
Atomic Structure and Electrical Activity of Grain Boundaries and Ruddlesden-Popper Faults in Cesium Lead Bromide Perovskite journal December 2018
Vapor-Phase Growth of CsPbBr 3 Microstructures for Highly Efficient Pure Green Light Emission journal December 2018
Recent advances in magnetic structure determination by neutron powder diffraction journal October 1993
ABINIT: First-principles approach to material and nanosystem properties journal December 2009
Recent developments in the ABINIT software package journal August 2016
The Renaissance of Halide Perovskites and Their Evolution as Emerging Semiconductors journal September 2015
Extraordinarily Stable Noncubic Structures of Au: A High-Pressure and -Temperature Study journal February 2017
Depressed Phase Transitions and Thermally Persistent Local Distortions in CsPbBr 3 Quantum Dots journal September 2018
Pressure Response of Photoluminescence in Cesium Lead Iodide Perovskite Nanocrystals journal April 2018
Pressure-Induced Structural Evolution and Optical Properties of Metal-Halide Perovskite CsPbCl 3 journal June 2018
Pressure-Induced Band Structure Evolution of Halide Perovskites: A First-Principles Atomic and Electronic Structure Study journal December 2018
Octahedral Rotation Preferences in Perovskite Iodides and Bromides journal February 2016
Pressure-Induced Structural and Optical Properties of Inorganic Halide Perovskite CsPbBr 3 journal July 2017
In Situ Raman Spectroscopic Studies of Thermal Stability of All-Inorganic Cesium Lead Halide (CsPbX 3 , X = Cl, Br, I) Perovskite Nanocrystals journal February 2019
Ruddlesden–Popper Phase in Two-Dimensional Inorganic Halide Perovskites: A Plausible Model and the Supporting Observations journal August 2017
Significantly Enhanced Emission Stability of CsPbBr 3 Nanocrystals via Chemically Induced Fusion Growth for Optoelectronic Devices journal October 2018
Coherent Nanotwins and Dynamic Disorder in Cesium Lead Halide Perovskite Nanocrystals journal April 2017
Highly Luminescent Phase-Stable CsPbI 3 Perovskite Quantum Dots Achieving Near 100% Absolute Photoluminescence Quantum Yield journal September 2017
High-Performance All-Inorganic CsPbCl 3 Perovskite Nanocrystal Photodetectors with Superior Stability journal February 2019
Crystal Growth of the Perovskite Semiconductor CsPbBr 3 : A New Material for High-Energy Radiation Detection journal June 2013
Pressure Effects on Structure and Optical Properties in Cesium Lead Bromide Perovskite Nanocrystals journal July 2017
Nanocrystals of Cesium Lead Halide Perovskites (CsPbX 3 , X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut journal February 2015
High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells journal July 2016
Low-threshold amplified spontaneous emission and lasing from colloidal nanocrystals of caesium lead halide perovskites journal August 2015
Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystals journal February 2018
On the crystal structure of colloidally prepared CsPbBr 3 quantum dots journal January 2016
Pressure-induced strong ferroelectric polarization in tetra-phase perovskite CsPbBr 3 journal January 2018
Effects of pressure on the ionic transport and photoelectrical properties of CsPbBr 3 journal February 2019
Reconstructing a solid-solid phase transformation pathway in CdSe nanosheets with associated soft ligands journal September 2010
Two-dimensional detector software: From real detector to idealised image or two-theta scan journal January 1996
Blue emitting organic semiconductors under high pressure: status and outlook journal April 2016
Special points for Brillouin-zone integrations journal June 1976
Photoluminescence of short-period GaAs/AlAs superlattices: A hydrostatic pressure and temperature study journal September 1998
Optimized norm-conserving Vanderbilt pseudopotentials journal August 2013
Interface Control of Emergent Ferroic Order in Ruddlesden-Popper Sr n + 1 Ti n O 3 n + 1 journal December 2011
Generalized Gradient Approximation Made Simple journal October 1996
High-pressure phases of group-IV, III–V, and II–VI compounds journal July 2003
EXPO2013 : a kit of tools for phasing crystal structures from powder data journal July 2013
Octahedral Tilting in Perovskites. I. Geometrical Considerations journal February 1997
Group-Theoretical Analysis of Octahedral Tilting in Perovskites journal December 1998
New compounds of the K 2 NIF 4 type journal August 1957
Structural Phase Transitions in CsPbBr 3 journal November 1974

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