Self-Assembly of Metallo-Supramolecules under Kinetic or Thermodynamic Control: Characterization of Positional Isomers Using Scanning Tunneling Spectroscopy

Wang, Lei; Song, Bo; Li, Yiming; Gong, Lele; Jiang, Xin; Wang, Ming; Lu, Shuai; Hao, Xin-Qi; Xia, Zhenhai; Zhang, Yuan; Hla, Saw Wai; Li, Xiaopeng

doi:10.1021/jacs.0c03459

Title: Self-Assembly of Metallo-Supramolecules under Kinetic or Thermodynamic Control: Characterization of Positional Isomers Using Scanning Tunneling Spectroscopy

Journal Article · Mon Apr 20 00:00:00 EDT 2020 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.0c03459· OSTI ID:1664385

^[1];

^[1]; Gong, Lele ^[2];

^[3];

^[3]; Lu, Shuai ^[4];

^[5];

^[2]; Zhang, Yuan ^[6];

^[7];

^[1]

Univ. of South Florida, Tampa, FL (United States)
Univ. of North Texas, Denton, TX (United States)
Jilin Univ. (China)
Univ. of South Florida, Tampa, FL (United States); Zhengzhou Univ. (China)
Zhengzhou Univ. (China)
Argonne National Lab. (ANL), Argonne, IL (United States); Old Dominion Univ., Norfolk, VA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Coordination-driven self-assembly has been extensively employed to construct a variety of discrete structures as a bottom-up strategy. However, mechanistic understanding regarding whether self-assembly is under kinetic or thermodynamic control is less explored. To date, such mechanistic investigation has been limited to distinct, assembled structures. It still remains a formidable challenge to study the kinetic and thermodynamic behavior of self-assembly systems with multiple assembled isomers due to the lack of characterization methods. Herein, we use a stepwise strategy which combined self-recognition and self-assembly processes to construct giant metallo-supramolecules with 8 positional isomers in solution. With the help of ultrahigh-vacuum, low-temperature scanning tunneling microscopy and scanning tunneling spectroscopy, we were able to unambiguously differentiate 14 isomers on the substrate which correspond to 8 isomers in solution. Through measurement of 162 structures, the experimental probability of each isomer was obtained and compared with the theoretical probability. Finally, such a comparison along with density functional theory (DFT) calculation suggested that although both kinetic and thermodynamic control existed in this self-assembly, the increased experimental probabilities of isomers compared to theoretical probabilities should be attributed to thermodynamic control.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Institutes of Health (NIH)

Grant/Contract Number:: AC02-06CH11357; R01GM128037

OSTI ID:: 1664385

Journal Information:: Journal of the American Chemical Society, Vol. 142, Issue 21; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Self-Assembly of Metallo-Supramolecules under Kinetic or Thermodynamic Control: Characterization of Positional Isomers Using Scanning Tunneling Spectroscopy

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