Strong absorption and ultrafast localisation in NaBiS2 nanocrystals with slow charge-carrier recombination

Yi-Teng Huang, Seán R. Kavanagh, Marcello Righetto, Marin Rusu, Igal Levine, Thomas Unold, Szymon J. Zelewski, Alexander J. Sneyd, Kaiwen Zhang, Linjie Dai, Andrew J. Britton, Junzhi Ye, Jaakko Julin, Mari Napari, Zhilong Zhang, James Xiao, Mikko Laitinen, Laura Torrente-Murciano, Samuel D. Stranks, Akshay Rao, Laura M. Herz, David O. Scanlon, Aron Walsh and Robert L. Z. Hoye ()
Additional contact information
Yi-Teng Huang: University of Cambridge
Seán R. Kavanagh: University College London
Marcello Righetto: University of Oxford, Clarendon Laboratory
Marin Rusu: Helmholtz-Zentrum Berlin für Materialien und Energie
Igal Levine: Helmholtz-Zentrum Berlin für Materialien und Energie GmbH
Thomas Unold: Helmholtz-Zentrum Berlin für Materialien und Energie
Szymon J. Zelewski: University of Cambridge
Alexander J. Sneyd: University of Cambridge
Kaiwen Zhang: University of Cambridge
Linjie Dai: University of Cambridge
Andrew J. Britton: University of Leeds
Junzhi Ye: University of Cambridge
Jaakko Julin: University of Jyväskylä
Mari Napari: University of Southampton
Zhilong Zhang: University of Cambridge
James Xiao: University of Cambridge
Mikko Laitinen: Technical University of Munich
Laura Torrente-Murciano: University of Cambridge
Samuel D. Stranks: University of Cambridge
Akshay Rao: University of Cambridge
Laura M. Herz: University of Oxford, Clarendon Laboratory
David O. Scanlon: University College London
Aron Walsh: Imperial College London
Robert L. Z. Hoye: Imperial College London

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

Abstract: Abstract I-V-VI2 ternary chalcogenides are gaining attention as earth-abundant, nontoxic, and air-stable absorbers for photovoltaic applications. However, the semiconductors explored thus far have slowly-rising absorption onsets, and their charge-carrier transport is not well understood yet. Herein, we investigate cation-disordered NaBiS2 nanocrystals, which have a steep absorption onset, with absorption coefficients reaching >105 cm−1 just above its pseudo-direct bandgap of 1.4 eV. Surprisingly, we also observe an ultrafast (picosecond-time scale) photoconductivity decay and long-lived charge-carrier population persisting for over one microsecond in NaBiS2 nanocrystals. These unusual features arise because of the localised, non-bonding S p character of the upper valence band, which leads to a high density of electronic states at the band edges, ultrafast localisation of spatially-separated electrons and holes, as well as the slow decay of trapped holes. This work reveals the critical role of cation disorder in these systems on both absorption characteristics and charge-carrier kinetics.

Date: 2022
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DOI: 10.1038/s41467-022-32669-3

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