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Dynamic Effects and Hydrogen Bonding in Mixed-Halide Perovskite Solar Cell Absorbers
Stockholm University, Faculty of Science, Department of Physics.
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Number of Authors: 162021 (English)In: The Journal of Physical Chemistry Letters, E-ISSN 1948-7185, Vol. 12, no 16, p. 3885-3890Article in journal (Refereed) Published
Abstract [en]

The organic component (methylammonium) of CH3NH3PbI3-xClx-based perovskites shows electronic hybridization with the inorganic framework via H-bonding between N and I sites. Femtosecond dynamics induced by core excitation are shown to strongly influence the measured X-ray emission spectra and the resonant inelastic soft X-ray scattering of the organic components. The N K core excitation leads to a greatly increased N-H bond length that modifies and strengthens the interaction with the inorganic framework compared to that in the ground state. The study indicates that excited-state dynamics must be accounted for in spectroscopic studies of this perovskite solar cell material, and the organic-inorganic hybridization interaction suggests new avenues for probing the electronic structure of this class of materials. It is incidentally shown that beam damage to the methylamine component can be avoided by moving the sample under the soft X-ray beam to minimize exposure and that this procedure is necessary to prevent the creation of experimental artifacts.

Place, publisher, year, edition, pages
2021. Vol. 12, no 16, p. 3885-3890
Keywords [en]
Ultrafast phenomena, Energy, Electronic structure, Resonance structures, Perovskites
National Category
Chemical Sciences Physical Sciences
Identifiers
URN: urn:nbn:se:su:diva-193696DOI: 10.1021/acs.jpclett.1c00745ISI: 000647271500003PubMedID: 33856793Scopus ID: 2-s2.0-85105061239OAI: oai:DiVA.org:su-193696DiVA, id: diva2:1565198
Available from: 2021-06-13 Created: 2021-06-13 Last updated: 2024-07-04Bibliographically approved
In thesis
1. In pursuit of next generation photovoltaics: An electronic structure study of emerging solar cell materials
Open this publication in new window or tab >>In pursuit of next generation photovoltaics: An electronic structure study of emerging solar cell materials
2022 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The development of a new generation of photovoltaic technologies is an important task in order to increase the production of clean energy. Perovskite solar cells, with an exceptionally rapid development over the last decade, have transformed into perhaps the most promising candidate to provide a low-cost alternative to conventional cells. While having excellent efficiency, the most successful category of photovoltaic perovskites, the class of hybrid lead-halide perovskites, suffers from poor stability in ambient conditions and gives rise to potential health concerns due to lead toxicity. Because of these issues, studies yielding a better understanding of lead-based perovskites and investigations of new, lead-free materials are likely meaningful steps towards better and more competitive solar cells. This thesis contains studies about established lead-based perovskites, CH3NH3PbI3 and CH(NH2)2PbI3, as well as the lead-free alternatives AgBi2I7 and Cs2AgBiI6. The main method employed is electronic structure calculations through density functional theory under periodic boundary conditions including band structure calculations and projected density of states. A particular focus is given to systems with mixed anion and related effects on the electronic structure.

Place, publisher, year, edition, pages
Stockholm: Department of Physics, Stockholm University, 2022. p. 74
Keywords
Solar cells, computational physics, density functional theory, electronic structure, molecular dynamics, Solceller, beräkningsfysik, täthetsfunktionalteori, elektronstruktur, molekyldynamik
National Category
Atom and Molecular Physics and Optics
Research subject
Theoretical Physics
Identifiers
urn:nbn:se:su:diva-202839 (URN)978-91-7911-818-1 (ISBN)978-91-7911-819-8 (ISBN)
Public defence
2022-04-29, room FB42, AlbaNova universitetscentrum, Roslagstullsbacken 21, Stockholm, 10:00 (Swedish)
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Supervisors
Available from: 2022-04-06 Created: 2022-03-15 Last updated: 2022-03-25Bibliographically approved

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Erbing, AxelYang, WanliOdelius, Michael

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