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A-site cation influence on the conduction band of lead bromide perovskites
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Condensed Matter Physics of Energy Materials. GJM Sci Consulting, Ft Lee, NJ 07024 USA..ORCID iD: 0000-0003-2932-7018
Stockholm Univ, AlbaNova Univ Ctr, Dept Phys, S-10691 Stockholm, Sweden.;Raja Ramanna Ctr Adv Technol, Theory & Simulat Lab, HRDS, Indore 452013, India.;Homi Bhabha Natl Inst, Training Sch Complex, Mumbai 400094, Maharashtra, India..
Deutsch Elektronen Synchrotron DESY, Notkestr 85, D-22607 Hamburg, Germany..
KTH Royal Inst Technol, Div Mat & Nano Phys, Dept Appl Phys, S-10691 Stockholm, Sweden..
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2022 (English)In: Nature Communications, E-ISSN 2041-1723, Vol. 13, no 1, article id 3839Article in journal (Refereed) Published
Abstract [en]

Hot carrier solar cells hold promise for exceeding the Shockley-Queisser limit. Slow hot carrier cooling is one of the most intriguing properties of lead halide perovskites and distinguishes this class of materials from competing materials used in solar cells. Here we use the element selectivity of high-resolution X-ray spectroscopy and density functional theory to uncover a previously hidden feature in the conduction band states, the sigma-pi energy splitting, and find that it is strongly influenced by the strength of electronic coupling between the A-cation and bromide-lead sublattice. Our finding provides an alternative mechanism to the commonly discussed polaronic screening and hot phonon bottleneck carrier cooling mechanisms. Our work emphasizes the optoelectronic role of the A-cation, provides a comprehensive view of A-cation effects in the crystal and electronic structures, and outlines a broadly applicable spectroscopic approach for assessing the impact of chemical alterations of the A-cation on perovskite electronic structure. The A-cation influence on the mechanism of slow hot carrier cooling in perovskites is controversial. Here, Man et al. resolve a debated issue regarding A-cation influence on the electronic structure of lead halide perovskites.

Place, publisher, year, edition, pages
Springer Nature, 2022. Vol. 13, no 1, article id 3839
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Materials Chemistry Physical Chemistry
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URN: urn:nbn:se:uu:diva-481380DOI: 10.1038/s41467-022-31416-yISI: 000820771400022PubMedID: 35787623OAI: oai:DiVA.org:uu-481380DiVA, id: diva2:1686826
Funder
Swedish Research Council, 2018-05525Swedish Research Council, 2018-06465Swedish Research Council, 2018-04330Swedish Research Council, 2018-05973Swedish Energy Agency, P50636Swedish Energy Agency, 2017-006797EU, Horizon 2020, 860553Available from: 2022-08-11 Created: 2022-08-11 Last updated: 2023-03-28Bibliographically approved

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Man, Gabriel J.Mukherjee, SohamRensmo, HåkanOdelius, MichaelButorin, Sergei
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