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Bandlike transport and charge-carrier dynamics in BiOI films

Bandlike transport and charge-carrier dynamics in BiOI films
Bandlike transport and charge-carrier dynamics in BiOI films

Following the emergence of lead halide perovskites (LHPs) as materials for efficient solar cells, research has progressed to explore stable, abundant, and nontoxic alternatives. However, the performance of such lead-free perovskite-inspired materials (PIMs) still lags significantly behind that of their LHP counterparts. For bismuth-based PIMs, one significant reason is a frequently observed ultrafast charge-carrier localization (or self-trapping), which imposes a fundamental limit on long-range mobility. Here we report the terahertz (THz) photoconductivity dynamics in thin films of BiOI and demonstrate a lack of such self-trapping, with good charge-carrier mobility, reaching ∼3 cm 2 V -1 s -1 at 295 K and increasing gradually to ∼13 cm 2 V -1 s -1 at 5 K, indicative of prevailing bandlike transport. Using a combination of transient photoluminescence and THz- and microwave-conductivity spectroscopy, we further investigate charge-carrier recombination processes, revealing charge-specific trapping of electrons at defects in BiOI over nanoseconds and low bimolecular band-to-band recombination. Subject to the development of passivation protocols, BiOI thus emerges as a superior light-harvesting semiconductor among the family of bismuth-based semiconductors.

1948-7185
6620-6629
Lal, Snigdha
6d52173b-a8fb-4cd0-b67a-926c75c46138
Righetto, Marcello
5514bef6-6c57-4bb2-ad0f-0143603fc265
Ulatowski, Aleksander M.
cbcf0d0e-0038-4719-8923-411370128dda
Motti, Silvia G.
17e505d8-5c5f-43e9-a5d3-370a0593e8f4
Sun, Zhuotong
60580679-fc41-4e65-b8b1-8928c57bb7b3
MacManus-Driscoll, Judith L.
e38446a4-e6e4-4123-a04c-10dde1e4e23f
Hoye, Robert L. Z.
18dfdd78-9a03-4a19-9bbe-590bdba6a13d
Herz, Laura M.
61d69096-5062-489f-b608-685166bc48f5
Lal, Snigdha
6d52173b-a8fb-4cd0-b67a-926c75c46138
Righetto, Marcello
5514bef6-6c57-4bb2-ad0f-0143603fc265
Ulatowski, Aleksander M.
cbcf0d0e-0038-4719-8923-411370128dda
Motti, Silvia G.
17e505d8-5c5f-43e9-a5d3-370a0593e8f4
Sun, Zhuotong
60580679-fc41-4e65-b8b1-8928c57bb7b3
MacManus-Driscoll, Judith L.
e38446a4-e6e4-4123-a04c-10dde1e4e23f
Hoye, Robert L. Z.
18dfdd78-9a03-4a19-9bbe-590bdba6a13d
Herz, Laura M.
61d69096-5062-489f-b608-685166bc48f5

Lal, Snigdha, Righetto, Marcello, Ulatowski, Aleksander M., Motti, Silvia G., Sun, Zhuotong, MacManus-Driscoll, Judith L., Hoye, Robert L. Z. and Herz, Laura M. (2023) Bandlike transport and charge-carrier dynamics in BiOI films. The Journal of Physical Chemistry Letters, 14 (29), 6620-6629. (doi:10.1021/acs.jpclett.3c01520).

Record type: Article

Abstract

Following the emergence of lead halide perovskites (LHPs) as materials for efficient solar cells, research has progressed to explore stable, abundant, and nontoxic alternatives. However, the performance of such lead-free perovskite-inspired materials (PIMs) still lags significantly behind that of their LHP counterparts. For bismuth-based PIMs, one significant reason is a frequently observed ultrafast charge-carrier localization (or self-trapping), which imposes a fundamental limit on long-range mobility. Here we report the terahertz (THz) photoconductivity dynamics in thin films of BiOI and demonstrate a lack of such self-trapping, with good charge-carrier mobility, reaching ∼3 cm 2 V -1 s -1 at 295 K and increasing gradually to ∼13 cm 2 V -1 s -1 at 5 K, indicative of prevailing bandlike transport. Using a combination of transient photoluminescence and THz- and microwave-conductivity spectroscopy, we further investigate charge-carrier recombination processes, revealing charge-specific trapping of electrons at defects in BiOI over nanoseconds and low bimolecular band-to-band recombination. Subject to the development of passivation protocols, BiOI thus emerges as a superior light-harvesting semiconductor among the family of bismuth-based semiconductors.

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Accepted/In Press date: 10 July 2023
e-pub ahead of print date: 18 July 2023
Published date: 18 July 2023
Additional Information: Funding Information: S.L. acknowledges funding from the Oxford India Centre for Sustainable Development. R.L.Z.H. thanks support from the Royal Academy of Engineering through the Research Fellowships Scheme (RF\201718\1701) and the Engineering and Physical Sciences Research Council (EPSRC), UK (EP/V014498/2). M.R., A.M.U., S.G.M., and L.M.H. acknowledge support by the Engineering and Physical Sciences Research Council (EPSRC), UK (EP/V010840/1, EP/S004947/1, EP/L016702/1). L.M.H. acknowledges support through a Hans Fischer Senior Fellowship from the Technical University of Munich’s Institute for Advanced Study, funded by the German Excellence Initiative. Publisher Copyright: © 2023 The Authors. Published by American Chemical Society

Identifiers

Local EPrints ID: 481116
URI: http://eprints.soton.ac.uk/id/eprint/481116
ISSN: 1948-7185
PURE UUID: c426d6f3-a3c9-446c-88fd-1f172bab721e
ORCID for Silvia G. Motti: ORCID iD orcid.org/0000-0002-8088-3485

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Date deposited: 16 Aug 2023 16:31
Last modified: 17 Mar 2024 04:17

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Contributors

Author: Snigdha Lal
Author: Marcello Righetto
Author: Aleksander M. Ulatowski
Author: Silvia G. Motti ORCID iD
Author: Zhuotong Sun
Author: Judith L. MacManus-Driscoll
Author: Robert L. Z. Hoye
Author: Laura M. Herz

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