Halide Perovskite-Lead Chalcohalide Nanocrystal Heterostructures

Muhammad Imran; Lucheng Peng; Andrea Pianetti; Valerio Pinchetti; Julien Ramade; Juliette Zito; Francesco Di Stasio; Joka Buha; Stefano Toso; Jun Song; Ivan Infante; Sara Bals; Sergio Brovelli; Liberato Manna

doi:10.1021/jacs.0c10916

Halide Perovskite-Lead Chalcohalide Nanocrystal Heterostructures

Muhammad Imran, Lucheng Peng, Andrea Pianetti, Valerio Pinchetti, Julien Ramade, Juliette Zito, Francesco Di Stasio, Joka Buha, Stefano Toso, Jun Song^*, Ivan Infante^*, Sara Bals^*, Sergio Brovelli^*, Liberato Manna^*

^*Corresponding author for this work

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

We report the synthesis of colloidal CsPbX3-Pb4S3Br2 (X = Cl, Br, I) nanocrystal heterostructures, providing an example of a sharp and atomically resolved epitaxial interface between a metal halide perovskite and a non-perovskite lattice. The CsPbBr3-Pb4S3Br2 nanocrystals are prepared by a two-step direct synthesis using preformed subnanometer CsPbBr3 clusters. Density functional theory calculations indicate the creation of a quasi-type II alignment at the heterointerface as well as the formation of localized trap states, promoting ultrafast separation of photogenerated excitons and carrier trapping, as confirmed by spectroscopic experiments. Postsynthesis reaction with either Cl- or I- ions delivers the corresponding CsPbCl3-Pb4S3Br2 and CsPbI3-Pb4S3Br2 heterostructures, thus enabling anion exchange only in the perovskite domain. An increased structural rigidity is conferred to the perovskite lattice when it is interfaced with the chalcohalide lattice. This is attested by the improved stability of the metastable γphase (or "black"phase) of CsPbI3 in the CsPbI3-Pb4S3Br2 heterostructure.

Original language	English
Pages (from-to)	1435-1446
Number of pages	12
Journal	Journal of the American Chemical Society
Volume	143
Issue number	3
Early online date	13 Jan 2021
DOIs	https://doi.org/10.1021/jacs.0c10916
Publication status	Published - 27 Jan 2021

Bibliographical note

Funding Information:
This work was performed on the Dutch national e-infrastructure with the support of SURF Cooperative. L.P. and J.S. are thankful for the support by the National Key R&D Program of China (2018YFC0910600) and the National Natural Science Foundation of China (61775145). F.D.S. and S.B. acknowledge support by the European Research Council via the ERC-StG “NANOLED” (851794) and the ERC-Cog “REALNANO” (815128). The authors acknowledge financial support from the European Commission under the Horizon 2020 Programme through Grant Agreement No. 731019 (EUSMI). S.B., A.P., and V.P. gratefully acknowledge the financial support from the Italian Ministry of University and Research (MIUR) through grant “Dipartimenti di Eccellenza-2017 Materials For Energy”.

Publisher Copyright:
© 2021 American Chemical Society. All rights reserved.

Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.

Funding

This work was performed on the Dutch national e-infrastructure with the support of SURF Cooperative. L.P. and J.S. are thankful for the support by the National Key R&D Program of China (2018YFC0910600) and the National Natural Science Foundation of China (61775145). F.D.S. and S.B. acknowledge support by the European Research Council via the ERC-StG “NANOLED” (851794) and the ERC-Cog “REALNANO” (815128). The authors acknowledge financial support from the European Commission under the Horizon 2020 Programme through Grant Agreement No. 731019 (EUSMI). S.B., A.P., and V.P. gratefully acknowledge the financial support from the Italian Ministry of University and Research (MIUR) through grant “Dipartimenti di Eccellenza-2017 Materials For Energy”.

Funders	Funder number
ERC-Cog
ERC-StG
Italian Ministry of University and Research
National Key R&D Program of China	2018YFC0910600
Horizon 2020 Framework Programme	815128, 731019, 851794
European Commission
European Research Council
National Natural Science Foundation of China	61775145
Ministero dell’Istruzione, dell’Università e della Ricerca

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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title = "Halide Perovskite-Lead Chalcohalide Nanocrystal Heterostructures",

abstract = "We report the synthesis of colloidal CsPbX3-Pb4S3Br2 (X = Cl, Br, I) nanocrystal heterostructures, providing an example of a sharp and atomically resolved epitaxial interface between a metal halide perovskite and a non-perovskite lattice. The CsPbBr3-Pb4S3Br2 nanocrystals are prepared by a two-step direct synthesis using preformed subnanometer CsPbBr3 clusters. Density functional theory calculations indicate the creation of a quasi-type II alignment at the heterointerface as well as the formation of localized trap states, promoting ultrafast separation of photogenerated excitons and carrier trapping, as confirmed by spectroscopic experiments. Postsynthesis reaction with either Cl- or I- ions delivers the corresponding CsPbCl3-Pb4S3Br2 and CsPbI3-Pb4S3Br2 heterostructures, thus enabling anion exchange only in the perovskite domain. An increased structural rigidity is conferred to the perovskite lattice when it is interfaced with the chalcohalide lattice. This is attested by the improved stability of the metastable γphase (or {"}black{"}phase) of CsPbI3 in the CsPbI3-Pb4S3Br2 heterostructure. ",

author = "Muhammad Imran and Lucheng Peng and Andrea Pianetti and Valerio Pinchetti and Julien Ramade and Juliette Zito and {Di Stasio}, Francesco and Joka Buha and Stefano Toso and Jun Song and Ivan Infante and Sara Bals and Sergio Brovelli and Liberato Manna",

note = "Funding Information: This work was performed on the Dutch national e-infrastructure with the support of SURF Cooperative. L.P. and J.S. are thankful for the support by the National Key R&D Program of China (2018YFC0910600) and the National Natural Science Foundation of China (61775145). F.D.S. and S.B. acknowledge support by the European Research Council via the ERC-StG “NANOLED” (851794) and the ERC-Cog “REALNANO” (815128). The authors acknowledge financial support from the European Commission under the Horizon 2020 Programme through Grant Agreement No. 731019 (EUSMI). S.B., A.P., and V.P. gratefully acknowledge the financial support from the Italian Ministry of University and Research (MIUR) through grant “Dipartimenti di Eccellenza-2017 Materials For Energy”. Publisher Copyright: {\textcopyright} 2021 American Chemical Society. All rights reserved. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.",

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AU - Imran, Muhammad

AU - Peng, Lucheng

AU - Pianetti, Andrea

AU - Pinchetti, Valerio

AU - Ramade, Julien

AU - Zito, Juliette

AU - Di Stasio, Francesco

AU - Buha, Joka

AU - Toso, Stefano

AU - Song, Jun

AU - Infante, Ivan

AU - Bals, Sara

AU - Brovelli, Sergio

AU - Manna, Liberato

N1 - Funding Information: This work was performed on the Dutch national e-infrastructure with the support of SURF Cooperative. L.P. and J.S. are thankful for the support by the National Key R&D Program of China (2018YFC0910600) and the National Natural Science Foundation of China (61775145). F.D.S. and S.B. acknowledge support by the European Research Council via the ERC-StG “NANOLED” (851794) and the ERC-Cog “REALNANO” (815128). The authors acknowledge financial support from the European Commission under the Horizon 2020 Programme through Grant Agreement No. 731019 (EUSMI). S.B., A.P., and V.P. gratefully acknowledge the financial support from the Italian Ministry of University and Research (MIUR) through grant “Dipartimenti di Eccellenza-2017 Materials For Energy”. Publisher Copyright: © 2021 American Chemical Society. All rights reserved. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.

PY - 2021/1/27

Y1 - 2021/1/27

N2 - We report the synthesis of colloidal CsPbX3-Pb4S3Br2 (X = Cl, Br, I) nanocrystal heterostructures, providing an example of a sharp and atomically resolved epitaxial interface between a metal halide perovskite and a non-perovskite lattice. The CsPbBr3-Pb4S3Br2 nanocrystals are prepared by a two-step direct synthesis using preformed subnanometer CsPbBr3 clusters. Density functional theory calculations indicate the creation of a quasi-type II alignment at the heterointerface as well as the formation of localized trap states, promoting ultrafast separation of photogenerated excitons and carrier trapping, as confirmed by spectroscopic experiments. Postsynthesis reaction with either Cl- or I- ions delivers the corresponding CsPbCl3-Pb4S3Br2 and CsPbI3-Pb4S3Br2 heterostructures, thus enabling anion exchange only in the perovskite domain. An increased structural rigidity is conferred to the perovskite lattice when it is interfaced with the chalcohalide lattice. This is attested by the improved stability of the metastable γphase (or "black"phase) of CsPbI3 in the CsPbI3-Pb4S3Br2 heterostructure.

AB - We report the synthesis of colloidal CsPbX3-Pb4S3Br2 (X = Cl, Br, I) nanocrystal heterostructures, providing an example of a sharp and atomically resolved epitaxial interface between a metal halide perovskite and a non-perovskite lattice. The CsPbBr3-Pb4S3Br2 nanocrystals are prepared by a two-step direct synthesis using preformed subnanometer CsPbBr3 clusters. Density functional theory calculations indicate the creation of a quasi-type II alignment at the heterointerface as well as the formation of localized trap states, promoting ultrafast separation of photogenerated excitons and carrier trapping, as confirmed by spectroscopic experiments. Postsynthesis reaction with either Cl- or I- ions delivers the corresponding CsPbCl3-Pb4S3Br2 and CsPbI3-Pb4S3Br2 heterostructures, thus enabling anion exchange only in the perovskite domain. An increased structural rigidity is conferred to the perovskite lattice when it is interfaced with the chalcohalide lattice. This is attested by the improved stability of the metastable γphase (or "black"phase) of CsPbI3 in the CsPbI3-Pb4S3Br2 heterostructure.

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Halide Perovskite-Lead Chalcohalide Nanocrystal Heterostructures

Abstract

Bibliographical note

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