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Self-assembly of a robust hydrogen-bonded octylphosphonate network on cesium lead bromide perovskite nanocrystals for light-emitting diodes

Self-assembly of a robust hydrogen-bonded octylphosphonate network on cesium lead bromide perovskite nanocrystals for light-emitting diodes
Self-assembly of a robust hydrogen-bonded octylphosphonate network on cesium lead bromide perovskite nanocrystals for light-emitting diodes
We report the self-assembly of an extensive inter-ligand hydrogen-bonding network of octylphosphonates on the surface of cesium lead bromide nanocrystals (CsPbBr3 NCs). The post-synthetic addition of octylphosphonic acid to oleic acid/oleylamine-capped CsPbBr3 NCs promoted the attachment of octylphosphonate to the NC surface, while the remaining oleylammonium ligands maintained the high dispersability of the NCs in non-polar solvent. Through powerful 2D solid-state 31P–1H NMR, we demonstrated that an ethyl acetate/acetonitrile purification regime was crucial for initiating the self-assembly of extensive octylphosphonate chains. Octylphosphonate ligands were found to preferentially bind in a monodentate mode through P–O−, leaving polar P[double bond, length as m-dash]O and P–OH groups free to form inter-ligand hydrogen bonds. The octylphosphonate ligand network strongly passivated the nanocrystal surface, yielding a fully-purified CsPbBr3 NC ink with PLQY of 62%, over 3 times higher than untreated NCs. We translated this to LED devices, achieving maximum external quantum efficiency and luminance of 7.74% and 1022 cd m−2 with OPA treatment, as opposed to 3.59% and 229 cd m−2 for untreated CsPbBr3 NCs. This represents one of the highest efficiency LEDs obtained for all-inorganic CsPbBr3 NCs, accomplished through simple, effective passivation and purification processes. The robust binding of octylphosphonates to the perovskite lattice, and specifically their ability to interlink through hydrogen bonding, offers a promising passivation approach which could potentially be beneficial across a breadth of halide perovskite optoelectronic applications.
2040-3364
12370-12380
Brown, Alasdair A.M.
3107ea0b-bebd-4b75-802e-9b65e28fcacf
Hooper, Thomas
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Veldhuis, Sjoerd
a6752a29-05de-4cac-9a2a-beda4dc9cecf
Chin, Xin Yu
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Bruno, Annalisa
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Vashishtha, Parth
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Tey, Ju Nie
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Jiang, Liudi
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Damodaran, Bahulayan
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Pu, Suan-Hui
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Mhaisalkar, Subodh
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Mathews, Nripan
c203a11f-0b0c-4ccf-b79d-b7b026253f3b
Brown, Alasdair A.M.
3107ea0b-bebd-4b75-802e-9b65e28fcacf
Hooper, Thomas
9f39fdda-2185-4b1f-a678-ac45d9d36748
Veldhuis, Sjoerd
a6752a29-05de-4cac-9a2a-beda4dc9cecf
Chin, Xin Yu
dd14be7d-dac9-450c-b854-e15639e9481c
Bruno, Annalisa
0075275b-4c20-4eb7-aed7-ab4766add0c0
Vashishtha, Parth
6e5532eb-f617-4afd-933e-890670fd039e
Tey, Ju Nie
e0ab0eac-f882-4da8-afbc-c3815d1e3ebf
Jiang, Liudi
374f2414-51f0-418f-a316-e7db0d6dc4d1
Damodaran, Bahulayan
9949c4ae-d4ae-40f1-981f-d4f7d3b57905
Pu, Suan-Hui
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Mhaisalkar, Subodh
edf3e5a0-cdc8-41f8-bd2a-902ad615d345
Mathews, Nripan
c203a11f-0b0c-4ccf-b79d-b7b026253f3b

Brown, Alasdair A.M., Hooper, Thomas, Veldhuis, Sjoerd, Chin, Xin Yu, Bruno, Annalisa, Vashishtha, Parth, Tey, Ju Nie, Jiang, Liudi, Damodaran, Bahulayan, Pu, Suan-Hui, Mhaisalkar, Subodh and Mathews, Nripan (2019) Self-assembly of a robust hydrogen-bonded octylphosphonate network on cesium lead bromide perovskite nanocrystals for light-emitting diodes. Nanoscale, 11 (25), 12370-12380. (doi:10.1039/C9NR02566A).

Record type: Article

Abstract

We report the self-assembly of an extensive inter-ligand hydrogen-bonding network of octylphosphonates on the surface of cesium lead bromide nanocrystals (CsPbBr3 NCs). The post-synthetic addition of octylphosphonic acid to oleic acid/oleylamine-capped CsPbBr3 NCs promoted the attachment of octylphosphonate to the NC surface, while the remaining oleylammonium ligands maintained the high dispersability of the NCs in non-polar solvent. Through powerful 2D solid-state 31P–1H NMR, we demonstrated that an ethyl acetate/acetonitrile purification regime was crucial for initiating the self-assembly of extensive octylphosphonate chains. Octylphosphonate ligands were found to preferentially bind in a monodentate mode through P–O−, leaving polar P[double bond, length as m-dash]O and P–OH groups free to form inter-ligand hydrogen bonds. The octylphosphonate ligand network strongly passivated the nanocrystal surface, yielding a fully-purified CsPbBr3 NC ink with PLQY of 62%, over 3 times higher than untreated NCs. We translated this to LED devices, achieving maximum external quantum efficiency and luminance of 7.74% and 1022 cd m−2 with OPA treatment, as opposed to 3.59% and 229 cd m−2 for untreated CsPbBr3 NCs. This represents one of the highest efficiency LEDs obtained for all-inorganic CsPbBr3 NCs, accomplished through simple, effective passivation and purification processes. The robust binding of octylphosphonates to the perovskite lattice, and specifically their ability to interlink through hydrogen bonding, offers a promising passivation approach which could potentially be beneficial across a breadth of halide perovskite optoelectronic applications.

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Accepted/In Press date: 31 May 2019
e-pub ahead of print date: 3 June 2019
Published date: 7 July 2019

Identifiers

Local EPrints ID: 433462
URI: http://eprints.soton.ac.uk/id/eprint/433462
ISSN: 2040-3364
PURE UUID: 62513886-45ab-4880-933f-3edb7b0899e5
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: 22 Aug 2019 16:30
Last modified: 26 Nov 2021 03:15

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Contributors

Author: Alasdair A.M. Brown ORCID iD
Author: Thomas Hooper
Author: Sjoerd Veldhuis
Author: Xin Yu Chin
Author: Annalisa Bruno
Author: Parth Vashishtha
Author: Ju Nie Tey
Author: Liudi Jiang ORCID iD
Author: Bahulayan Damodaran
Author: Suan-Hui Pu ORCID iD
Author: Subodh Mhaisalkar
Author: Nripan Mathews

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