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Control Over the Microstructure of Vapor‐Deposited CsPbBr 3 Enhances Amplified Spontaneous Emission

Abstract:
Inorganic cesium‐based metal halide perovskite (MHP) semiconductors have great potential as active layers in optoelectronic devices, such as perovskite light‐emitting diodes (PeLEDs) and perovskite lasers. However, precise control of crystal type, quality, and thickness is required to create high‐performance and reproducible devices. Vapor‐phase vacuum deposition enables fabrication of MHP thin films and devices with excellent uniformity and control over layer thickness, although a full understanding of crystal growth mechanisms and products has proved elusive. Here, conditions of vapor co‐deposition of CsBr and PbBr are related with the optical performance and atomic microstructure of resulting CsPbBr3 thin films. It is found that the structure is predominantly photoactive γ‐CsPbBr3 over a wide range of conditions, but the presence of impurity phases and Ruddlesden–Popper (RP) planar defects both degrade optical performance as quantified through measured amplified spontaneous emission (ASE) thresholds. Furthermore, the atomic structure of the dominant impurity phases is resolved: CsPb2Br5 and Cs4PbBr6. It is revealed that a small nominal excess of CsBr‐precursor flux during co‐evaporation can significantly enhance the nucleation of thin films, resulting in well‐defined grains greater than 500 nm in size and the relative suppression of RP planar defects. Such films exhibit intensified photoluminescence (PL) emission and a reduced ASE threshold of 30.9 µJ cm−2.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1002/adom.202502160

Authors


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Institution:
University of Oxford
Role:
Author
ORCID:
0000-0002-1335-4073
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Role:
Author
ORCID:
0009-0003-5300-3272
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Institution:
University of Oxford
Role:
Author
ORCID:
0009-0008-0136-6086
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Institution:
University of Oxford
Role:
Author
ORCID:
0000-0002-9726-0436
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Institution:
University of Oxford
Role:
Author
ORCID:
0000-0001-9621-334X


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Funder identifier:
https://ror.org/05mmh0f86
More from this funder
Funder identifier:
https://ror.org/012mzw131


Publisher:
Wiley
Journal:
Advanced Optical Materials More from this journal
Article number:
e02160
Publication date:
2025-09-28
DOI:
EISSN:
2195-1071
ISSN:
2195-1071


Language:
English
Keywords:
Source identifiers:
3323572
Deposit date:
2025-09-29
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