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In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication

Xin Huang, Jinlong Zhu, Binghui Ge, Frauke Gerdes, Christian Klinke Orcid Logo, Zhongwu Wang

Journal of the American Chemical Society, Volume: 143, Issue: 11, Pages: 4234 - 4243

Swansea University Author: Christian Klinke Orcid Logo

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DOI (Published version): 10.1021/jacs.0c12087

Abstract

Crystallization and growth of anisotropic nanocrystals (NCs) into distinct superlattices were studied in real time, yielding kinetic details and designer parameters for scale-up fabrication of functional materials. Using octahedral PbS NC blocks, we discovered that NC assembly involves a primary lam...

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Published in: Journal of the American Chemical Society
ISSN: 0002-7863 1520-5126
Published: American Chemical Society (ACS) 2021
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URI: https://cronfa.swan.ac.uk/Record/cronfa56730
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first_indexed 2021-04-25T10:27:03Z
last_indexed 2021-08-10T03:15:16Z
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spelling 2021-08-09T15:11:42.9457588 v2 56730 2021-04-25 In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication c10c44238eabfb203111f88a965f5372 0000-0001-8558-7389 Christian Klinke Christian Klinke true false 2021-04-25 CHEM Crystallization and growth of anisotropic nanocrystals (NCs) into distinct superlattices were studied in real time, yielding kinetic details and designer parameters for scale-up fabrication of functional materials. Using octahedral PbS NC blocks, we discovered that NC assembly involves a primary lamellar ordering of NC-detached Pb(OA)2 molecules on the front-spreading solvent surfaces. Upon a spontaneous increase of NC concentration during solvent processing, PbS NCs preferentially self-assembled into an orientation-disordered face-centered cubic (fcc) superlattice, which subsequently transformed into a body-centered cubic (bcc) superlattice with single NC-orientational ordering across individual domains. Unlike the deformation-based transformation route claimed previously, this solid–solid phase transformation involved a hidden intermediate formation of a lamellar-confined liquid interface at cost of the disassembly (melting) of small fcc grains. Such highly condensed and liquidized NCs recrystallized into the stable bcc phase with an energy reduction of 1.16 kBT. This energy-favorable and high NC-fraction-driven bcc phase grew as a 2D film at a propagation rate of 0.74 μm/min, smaller than the 1.23 μm/min observed in the early nucleated fcc phase under a dilute NC environment. Taking such insights and defined parameters, we designed experiments to manipulate the NC assembly pathway and achieved scalable fabrication of a large/single bcc supercrystal with coherent ordering of NC translation and atomic plane orientation. This study not only provides a design avenue for controllable fabrication of a large supercrystal with desired superlattices for application but also sheds new light on the nature of crystal nucleation/growth and phase transformation by extending the lengths from the nanoscale into the atomic scale, molecular scale, and microscale levels. Journal Article Journal of the American Chemical Society 143 11 4234 4243 American Chemical Society (ACS) 0002-7863 1520-5126 24 3 2021 2021-03-24 10.1021/jacs.0c12087 COLLEGE NANME Chemistry COLLEGE CODE CHEM Swansea University 2021-08-09T15:11:42.9457588 2021-04-25T11:24:14.9696874 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemistry Xin Huang 1 Jinlong Zhu 2 Binghui Ge 3 Frauke Gerdes 4 Christian Klinke 0000-0001-8558-7389 5 Zhongwu Wang 6
title In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication
spellingShingle In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication
Christian Klinke
title_short In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication
title_full In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication
title_fullStr In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication
title_full_unstemmed In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication
title_sort In Situ Constructing the Kinetic Roadmap of Octahedral Nanocrystal Assembly Toward Controlled Superlattice Fabrication
author_id_str_mv c10c44238eabfb203111f88a965f5372
author_id_fullname_str_mv c10c44238eabfb203111f88a965f5372_***_Christian Klinke
author Christian Klinke
author2 Xin Huang
Jinlong Zhu
Binghui Ge
Frauke Gerdes
Christian Klinke
Zhongwu Wang
format Journal article
container_title Journal of the American Chemical Society
container_volume 143
container_issue 11
container_start_page 4234
publishDate 2021
institution Swansea University
issn 0002-7863
1520-5126
doi_str_mv 10.1021/jacs.0c12087
publisher American Chemical Society (ACS)
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemistry{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemistry
document_store_str 0
active_str 0
description Crystallization and growth of anisotropic nanocrystals (NCs) into distinct superlattices were studied in real time, yielding kinetic details and designer parameters for scale-up fabrication of functional materials. Using octahedral PbS NC blocks, we discovered that NC assembly involves a primary lamellar ordering of NC-detached Pb(OA)2 molecules on the front-spreading solvent surfaces. Upon a spontaneous increase of NC concentration during solvent processing, PbS NCs preferentially self-assembled into an orientation-disordered face-centered cubic (fcc) superlattice, which subsequently transformed into a body-centered cubic (bcc) superlattice with single NC-orientational ordering across individual domains. Unlike the deformation-based transformation route claimed previously, this solid–solid phase transformation involved a hidden intermediate formation of a lamellar-confined liquid interface at cost of the disassembly (melting) of small fcc grains. Such highly condensed and liquidized NCs recrystallized into the stable bcc phase with an energy reduction of 1.16 kBT. This energy-favorable and high NC-fraction-driven bcc phase grew as a 2D film at a propagation rate of 0.74 μm/min, smaller than the 1.23 μm/min observed in the early nucleated fcc phase under a dilute NC environment. Taking such insights and defined parameters, we designed experiments to manipulate the NC assembly pathway and achieved scalable fabrication of a large/single bcc supercrystal with coherent ordering of NC translation and atomic plane orientation. This study not only provides a design avenue for controllable fabrication of a large supercrystal with desired superlattices for application but also sheds new light on the nature of crystal nucleation/growth and phase transformation by extending the lengths from the nanoscale into the atomic scale, molecular scale, and microscale levels.
published_date 2021-03-24T04:11:54Z
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score 11.035874

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