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Aerosol-Assisted Crystallization Lowers Intrinsic Quantum Confinement and Improves Optoelectronic Performance in FAPbI 3 Films

Abstract:
FAPbI3 has emerged as a promising semiconductor for photovoltaic applications offering a suitable bandgap for single-junction cells and high chemical stability. However, device efficiency is negatively affected by intrinsic quantum confinement (QC) effects that manifest as additional peaks in the absorption spectra. Here, we show that aerosol-assisted crystallization is an effective method to improve crystallinity and suppresses regions exhibiting QC in FAPbI3. We demonstrate that films with minimized QC effects exhibit markedly enhanced optoelectronic properties, such as higher charge-carrier mobilities and recombination lifetimes. Films crystallized under an aerosol solvent flow of either a mixture of N, N-dimethylformamide and dimethyl sulfoxide or methylammonium thiocyanate vapor displayed reduced charge-carrier recombination losses and improved diffusion lengths compared to those of thermally annealed control films. Our study indicates clear correlations between suppression of QC features in absorption spectra with optimization of crystallinity and mitigation of internal strain, highlighting pathways toward high-performance solar cells.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/acs.jpclett.5c00041

Authors


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Institution:
University of Oxford
Division:
MPLS
Department:
Physics
Sub department:
Physics - Central
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Physics
Sub department:
Physics - Central
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Physics
Sub department:
Physics - Central
Role:
Author
ORCID:
0000-0002-7707-1611
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Physics
Sub department:
Physics - Central
Role:
Author
ORCID:
0000-0002-0301-8033


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


Publisher:
American Chemical Society
Journal:
The Journal of Physical Chemistry Letters More from this journal
Volume:
16
Issue:
9
Pages:
2212-2222
Publication date:
2025-02-21
Acceptance date:
2025-02-14
DOI:
EISSN:
1948-7185


Language:
English
Source identifiers:
2745979
Deposit date:
2025-03-07
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