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Sensitivity of Nitrogen K-Edge X-ray Absorption to Halide Substitution and Thermal Fluctuations in Methylammonium Lead-Halide Perovskites
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0001-9518-9405
Stockholm University, Faculty of Science, Department of Physics. Raja Ramanna Centre for Advanced Technology, India.ORCID iD: 0000-0002-4546-8219
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Number of Authors: 122021 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 125, no 15, p. 8360-8368Article in journal (Refereed) Published
Abstract [en]

The performance of hybrid perovskite materials in solar cells crucially depends on their electronic properties, and it is important to investigate contributions to the total electronic structure from specific components in the material. In a combined theoretical and experimental study of CH3NH3PbI3-methylammonium lead triiodide (MAPI)-and its bromide cousin CH3NH3PbBr3 (MAPB), we analyze nitrogen K-edge (N Is-to-2p*) X-ray absorption (XA) spectra measured in MAPI and MAPB single crystals. This permits comparison of spectral features to the local character of unoccupied molecular orbitals on the CH3NH3+ (MA(+)) counterions and allows us to investigate how thermal fluctuations, hydrogen bonding, and halide-ion substitution influence the XA spectra as a measure of the local electronic structure. In agreement with the experiment, the simulated spectra for MAPI and MAPB show close similarity, except that the MAPB spectral features are blue-shifted by +0.31 eV. The shift is shown to arise from the intrinsic difference in the electronic structure of the two halide atoms rather than from structural differences between the materials. In addition, from the spectral sampling analysis of molecular dynamics simulations, clear correlations between geometric descriptors(N-C, N-H, and H center dot center dot center dot I/Br distances) and spectral features are identified and used to explain the spectral shapes.

Place, publisher, year, edition, pages
2021. Vol. 125, no 15, p. 8360-8368
Keywords [en]
Crystal structure, Ions, Nitrogen, Noncovalent interactions, Mathematical methods
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:su:diva-194122DOI: 10.1021/acs.jpcc.1c02017ISI: 000644438400036OAI: oai:DiVA.org:su-194122DiVA, id: diva2:1567393
Available from: 2021-06-16 Created: 2021-06-16 Last updated: 2022-11-29Bibliographically approved
In thesis
1. Modeling hybrid halide perovskites for solar cell applications: Simulations of electronic structure and X-ray spectroscopy
Open this publication in new window or tab >>Modeling hybrid halide perovskites for solar cell applications: Simulations of electronic structure and X-ray spectroscopy
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Over the past 13 years, perovskites have become a very promising candidate in the search for cheap and effective photovoltaic materials for solar cells.  Perovskite solar cell power conversion efficiency has increased from 3.8% in 2009 to over 25% by late 2022, rivaling that of crystalline silicon cells, and there are a variety of potential chemical compositions that provide a range of materials to investigate.  However, there are still questions about the specific role of all the different chemical components in the material and how they influence its efficiency.  This thesis aims to investigate the effect of material composition and structure through electronic structure calculations and theoretical X-ray absorption and X-ray photoelectron spectroscopy, with comparison to experimental spectra.  Herein, studies on the prototypical hybrid halide perovskite methylammonium lead triiodide (CH3NH3PbI3) are presented and compared among materials with various differences: structural/elemental changes in the case of its precursor methylammonium iodide (CH3NH3I), halide substitution in the case of methylammonium lead tribromide (CH3NH3PbBr3), or organic cation substitution in the case of formamidinium lead triiodide (CH(NH2)2PbI3).

Place, publisher, year, edition, pages
Stockholm: Department of Physics, Stockholm University, 2022. p. 54
Keywords
Solar cells, perovskites, computational chemistry, simulations, electronic structure, density functional theory, X-ray spectroscopy
National Category
Atom and Molecular Physics and Optics
Research subject
Chemical Physics
Identifiers
urn:nbn:se:su:diva-211949 (URN)978-91-8014-114-7 (ISBN)978-91-8014-115-4 (ISBN)
Public defence
2023-01-13, Lärosal 14, Albano Hus 2, Albanovägen 18, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
Swedish Energy Agency, 2017-006797
Available from: 2022-12-20 Created: 2022-11-29 Last updated: 2022-12-12Bibliographically approved

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Sterling, Cody M.Kamal, ChinnathambiOdelius, Michael

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