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Precise control of CsPbBr3 perovskite nanocrystal growth at room temperature: size tunability and synthetic insights

Precise control of CsPbBr3 perovskite nanocrystal growth at room temperature: size tunability and synthetic insights
Precise control of CsPbBr3 perovskite nanocrystal growth at room temperature: size tunability and synthetic insights
Room-temperature perovskite nanocrystal syntheses have previously lacked the size tunability attainable through high-temperature methods. Herein, we outline a scalable approach whereby the nucleation and growth of CsPbBr3 nanocrystals (NCs) can be decoupled and controlled at room temperature by utilizing different ligands. We employed octylphosphonic acid (OPA) ligands to regulate the critical radius and the NC growth rate. The subsequent addition of a bulkier didodecyldimethylammonium bromide ligand quenches the NC growth, defining the reaction duration. Management of these three variables enables precise tuning of the NC diameter between 6.8 and 13.6 nm. The photoluminescence quantum yield of the NCs remains above 80% for all sizes even after thorough antisolvent purification. The use of hydrogen-bonding OPA ligands enhances quantum confinement effects, characterized by strong, well-resolved absorption peaks. Solution and solid-state nuclear magnetic resonance spectra confirmed the effective removal of unbound ligands during purification and the presence of a hydrogen-bonded network of OPA ligands on the surface of the purified NCs. Overall, this approach has the potential to facilitate a broad range of future endeavors from studies of hot carrier dynamics to both optically and electrically driven device applications.
0897-4756
2387-2397
Brown, Alasdair A.M.
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Vashishtha, Parth
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Hooper, Thomas J.N.
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Ng, Yan Fong
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Nutan, Gautam V.
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Fang, Yanan
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Giovanni, David
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Tey, Ju Nie
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Jiang, Liudi
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Damodaran, Bahulayan
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Sum, Tze Chien
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Pu, Suan Hui
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Mhaisalkar, Subodh G.
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Mathews, Nripan
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Brown, Alasdair A.M.
3107ea0b-bebd-4b75-802e-9b65e28fcacf
Vashishtha, Parth
6e5532eb-f617-4afd-933e-890670fd039e
Hooper, Thomas J.N.
ecfdf81c-ac2e-48d7-aea1-096555d0b917
Ng, Yan Fong
08858c56-c5c4-4adf-b96f-e2a1bdcfbbea
Nutan, Gautam V.
dcacad82-dc46-4969-8096-e4d374562b16
Fang, Yanan
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Giovanni, David
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Tey, Ju Nie
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Jiang, Liudi
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Damodaran, Bahulayan
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Sum, Tze Chien
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Pu, Suan Hui
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Mhaisalkar, Subodh G.
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Mathews, Nripan
c203a11f-0b0c-4ccf-b79d-b7b026253f3b

Brown, Alasdair A.M., Vashishtha, Parth, Hooper, Thomas J.N., Ng, Yan Fong, Nutan, Gautam V., Fang, Yanan, Giovanni, David, Tey, Ju Nie, Jiang, Liudi, Damodaran, Bahulayan, Sum, Tze Chien, Pu, Suan Hui, Mhaisalkar, Subodh G. and Mathews, Nripan (2021) Precise control of CsPbBr3 perovskite nanocrystal growth at room temperature: size tunability and synthetic insights. Chemistry of Materials, 33 (7), 2387-2397. (doi:10.1021/acs.chemmater.0c04569).

Record type: Article

Abstract

Room-temperature perovskite nanocrystal syntheses have previously lacked the size tunability attainable through high-temperature methods. Herein, we outline a scalable approach whereby the nucleation and growth of CsPbBr3 nanocrystals (NCs) can be decoupled and controlled at room temperature by utilizing different ligands. We employed octylphosphonic acid (OPA) ligands to regulate the critical radius and the NC growth rate. The subsequent addition of a bulkier didodecyldimethylammonium bromide ligand quenches the NC growth, defining the reaction duration. Management of these three variables enables precise tuning of the NC diameter between 6.8 and 13.6 nm. The photoluminescence quantum yield of the NCs remains above 80% for all sizes even after thorough antisolvent purification. The use of hydrogen-bonding OPA ligands enhances quantum confinement effects, characterized by strong, well-resolved absorption peaks. Solution and solid-state nuclear magnetic resonance spectra confirmed the effective removal of unbound ligands during purification and the presence of a hydrogen-bonded network of OPA ligands on the surface of the purified NCs. Overall, this approach has the potential to facilitate a broad range of future endeavors from studies of hot carrier dynamics to both optically and electrically driven device applications.

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2021 Precise Control of CsPbBr3 Perovskite Nanocrystal Growth at Rm Temp acs.chemmater.0c04569 - Version of Record
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Accepted/In Press date: 16 March 2021
e-pub ahead of print date: 29 March 2021
Published date: 13 April 2021

Identifiers

Local EPrints ID: 487824
URI: http://eprints.soton.ac.uk/id/eprint/487824
ISSN: 0897-4756
PURE UUID: de4b98a7-1a4d-456f-ae4a-c0cd82ff32f1
ORCID for Alasdair A.M. Brown: ORCID iD orcid.org/0000-0002-0714-3851
ORCID for Liudi Jiang: ORCID iD orcid.org/0000-0002-3400-825X
ORCID for Suan Hui Pu: ORCID iD orcid.org/0000-0002-3335-8880

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Date deposited: 05 Mar 2024 18:50
Last modified: 02 Nov 2024 02:57

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Contributors

Author: Alasdair A.M. Brown ORCID iD
Author: Parth Vashishtha
Author: Thomas J.N. Hooper
Author: Yan Fong Ng
Author: Gautam V. Nutan
Author: Yanan Fang
Author: David Giovanni
Author: Ju Nie Tey
Author: Liudi Jiang ORCID iD
Author: Bahulayan Damodaran
Author: Tze Chien Sum
Author: Suan Hui Pu ORCID iD
Author: Subodh G. Mhaisalkar
Author: Nripan Mathews

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