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Sensitivity of Nitrogen K-Edge X-ray Absorption to Halide Substitution and Thermal Fluctuations in Methylammonium Lead-Halide Perovskites
Stockholm Univ, Dept Phys, SE-10691 Stockholm, Sweden.
Stockholm Univ, Dept Phys, SE-10691 Stockholm, Sweden; Raja Ramanna Ctr Adv Technol, Theory & Simulat Lab, HRDS, Indore 452013, Madhya Pradesh, India.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Condensed Matter Physics of Energy Materials.ORCID iD: 0000-0003-2932-7018
Tata Inst Fundamental Res, TIFR Ctr Interdisciplinary Sci, Hyderabad 500046, India.
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2021 (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 1s-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···I/Br distances) and spectral features are identified and used to explain the spectral shapes.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2021. Vol. 125, no 15, p. 8360-8368
National Category
Materials Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-443963DOI: 10.1021/acs.jpcc.1c02017ISI: 000644438400036PubMedID: 34084262OAI: oai:DiVA.org:uu-443963DiVA, id: diva2:1563643
Funder
Swedish Research Council, 2018-07152Swedish Research Council, 2018-05973Swedish Research Council, 2018-06465Swedish Research Council, 2018-04330Swedish Research Council, 2018-05525Swedish Research Council, 2015-03956Swedish Research Council, 2016-04590Swedish Energy Agency, P43549-1Swedish Energy Agency, 2017-006797Swedish Foundation for Strategic Research, RMA15-0130EU, Horizon 2020, 730872Vinnova, 2018-04969Swedish Research Council Formas, 2019-02496EU, Horizon 2020, 860553Swedish National Infrastructure for Computing (SNIC)Carl Tryggers foundation Göran Gustafsson Foundation for promotion of scientific research at Uppala University and Royal Institute of TechnologyAvailable from: 2021-06-10 Created: 2021-06-10 Last updated: 2024-06-04Bibliographically approved

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