A-site cation influence on the conduction band of lead bromide perovskites

Gabriel J. Man (), Chinnathambi Kamal, Aleksandr Kalinko, Dibya Phuyal, Joydev Acharya, Soham Mukherjee, Pabitra K. Nayak, Håkan Rensmo, Michael Odelius and Sergei M. Butorin ()
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Gabriel J. Man: Uppsala University
Chinnathambi Kamal: Stockholm University, AlbaNova University Center
Aleksandr Kalinko: Deutsches Elektronen-Synchrotron DESY
Dibya Phuyal: KTH Royal Institute of Technology
Joydev Acharya: Gopanpally Village, Serilingampally Mandal
Soham Mukherjee: Uppsala University
Pabitra K. Nayak: Gopanpally Village, Serilingampally Mandal
Håkan Rensmo: Uppsala University
Michael Odelius: Stockholm University, AlbaNova University Center
Sergei M. Butorin: Uppsala University

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract 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 σ-π 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.

Date: 2022
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DOI: 10.1038/s41467-022-31416-y

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