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Title: Thermally-induced reversible structural isomerization in colloidal semiconductor CdS magic-size clusters

Abstract

Structural isomerism of colloidal semiconductor nanocrystals has been largely unexplored. Here, we report one pair of structural isomers identified for colloidal nanocrystals which exhibit thermally-induced reversible transformations behaving like molecular isomerization. The two isomers are CdS magic-size clusters with sharp absorption peaks at 311 and 322 nm. They have identical cluster masses, but slightly different structures. Furthermore, their interconversions follow first-order unimolecular reaction kinetics. We anticipate that such isomeric kinetics are applicable to a variety of small-size functional nanomaterials, and that the methodology developed for our kinetic study will be helpful to investigate and exploit solid-solid transformations in other semiconductor nanocrystals. Furthermore, the findings on structural isomerism should stimulate attention toward advanced design and synthesis of functional nanomaterials enabled by structural transformations.

Authors:
 [1];  [1];  [2];  [3];  [1];  [2];  [4];  [5];  [6];  [6];  [1];  [7];  [1]
  1. Sichuan Univ., Chengdu (People's Republic of China)
  2. Huazhong Univ. of Science & Technology, Wuhan (People's Republic of China)
  3. National Research Council of Canada, Ottawa, ON (Canada)
  4. Queen Mary Univ. of London, London (United Kingdom)
  5. Queen Mary Univ. of London, London (United Kingdom); Sichuan Univ., Chengdu (People's Republic of China)
  6. Argonne National Lab. (ANL), Lemont, IL (United States)
  7. Chinese Academy of Sciences, Shanghai (China)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Natural Science Foundation of China (NNSFC); Fundamental Research Funds for the Central Universities; USDOE
OSTI Identifier:
1466370
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS

Citation Formats

Zhang, Baowei, Zhu, Tingting, Ou, Mingyang, Rowell, Nelson, Fan, Hongsong, Han, Jiantao, Tan, Lei, Dove, Martin T., Ren, Yang, Zuo, Xiaobing, Han, Shuo, Zeng, Jianrong, and Yu, Kui. Thermally-induced reversible structural isomerization in colloidal semiconductor CdS magic-size clusters. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04842-0.
Zhang, Baowei, Zhu, Tingting, Ou, Mingyang, Rowell, Nelson, Fan, Hongsong, Han, Jiantao, Tan, Lei, Dove, Martin T., Ren, Yang, Zuo, Xiaobing, Han, Shuo, Zeng, Jianrong, & Yu, Kui. Thermally-induced reversible structural isomerization in colloidal semiconductor CdS magic-size clusters. United States. doi:10.1038/s41467-018-04842-0.
Zhang, Baowei, Zhu, Tingting, Ou, Mingyang, Rowell, Nelson, Fan, Hongsong, Han, Jiantao, Tan, Lei, Dove, Martin T., Ren, Yang, Zuo, Xiaobing, Han, Shuo, Zeng, Jianrong, and Yu, Kui. Wed . "Thermally-induced reversible structural isomerization in colloidal semiconductor CdS magic-size clusters". United States. doi:10.1038/s41467-018-04842-0. https://www.osti.gov/servlets/purl/1466370.
@article{osti_1466370,
title = {Thermally-induced reversible structural isomerization in colloidal semiconductor CdS magic-size clusters},
author = {Zhang, Baowei and Zhu, Tingting and Ou, Mingyang and Rowell, Nelson and Fan, Hongsong and Han, Jiantao and Tan, Lei and Dove, Martin T. and Ren, Yang and Zuo, Xiaobing and Han, Shuo and Zeng, Jianrong and Yu, Kui},
abstractNote = {Structural isomerism of colloidal semiconductor nanocrystals has been largely unexplored. Here, we report one pair of structural isomers identified for colloidal nanocrystals which exhibit thermally-induced reversible transformations behaving like molecular isomerization. The two isomers are CdS magic-size clusters with sharp absorption peaks at 311 and 322 nm. They have identical cluster masses, but slightly different structures. Furthermore, their interconversions follow first-order unimolecular reaction kinetics. We anticipate that such isomeric kinetics are applicable to a variety of small-size functional nanomaterials, and that the methodology developed for our kinetic study will be helpful to investigate and exploit solid-solid transformations in other semiconductor nanocrystals. Furthermore, the findings on structural isomerism should stimulate attention toward advanced design and synthesis of functional nanomaterials enabled by structural transformations.},
doi = {10.1038/s41467-018-04842-0},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {6}
}

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Cited by: 15 works
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    Discontinuous Growth of II−VI Semiconductor Nanocrystals from Different Materials
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    • Zanella, Marco; Abbasi, Azhar Z.; Schaper, Andreas K.
    • The Journal of Physical Chemistry C, Vol. 114, Issue 14
    • DOI: 10.1021/jp906812t

    A Generic Method for Rational Scalable Synthesis of Monodisperse Metal Sulfide Nanocrystals
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    CdS Magic-Sized Nanocrystals Exhibiting Bright Band Gap Photoemission via Thermodynamically Driven Formation
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    • DOI: 10.1038/nature22389

    Solid–solid phase transitions via melting in metals
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    Polymorphism in magic-sized Au144(SR)60 clusters
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    • Jensen, Kirsten M. Ø.; Juhas, Pavol; Tofanelli, Marcus A.
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms11859

    General low-temperature reaction pathway from precursors to monomers before nucleation of compound semiconductor nanocrystals
    journal, August 2016

    • Yu, Kui; Liu, Xiangyang; Qi, Ting
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms12223

    Optical determination of crystal phase in semiconductor nanocrystals
    journal, May 2017

    • Lim, Sung Jun; Schleife, André; Smith, Andrew M.
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14849

    Probing intermediates of the induction period prior to nucleation and growth of semiconductor quantum dots
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    • Liu, Mingyang; Wang, Kun; Wang, Linxi
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms15467

    The mechanism of ultrafast structural switching in superionic copper (I) sulphide nanocrystals
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    • Miller, T. A.; Wittenberg, J. S.; Wen, H.
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