Evolution from unimolecular to colloidal-quantum-dot-like character in chlorine or zinc incorporated InP magic size clusters

Yongju Kwon, Juwon Oh, Eunjae Lee, Sang Hyeon Lee, Anastasia Agnes, Gyuhyun Bang, Jeongmin Kim, Dongho Kim () and Sungjee Kim ()
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Yongju Kwon: Department of Chemistry, Pohang University of Science and Technology
Juwon Oh: Department of Chemistry and Spectroscopy Laboratory for Functional π-Electronic Systems, Yonsei University
Eunjae Lee: Department of Chemistry, Pohang University of Science and Technology
Sang Hyeon Lee: Department of Chemistry and Spectroscopy Laboratory for Functional π-Electronic Systems, Yonsei University
Anastasia Agnes: Department of Chemistry, Pohang University of Science and Technology
Gyuhyun Bang: Department of Chemistry, Pohang University of Science and Technology
Jeongmin Kim: Department of Chemistry, Pohang University of Science and Technology
Dongho Kim: Department of Chemistry and Spectroscopy Laboratory for Functional π-Electronic Systems, Yonsei University
Sungjee Kim: Department of Chemistry, Pohang University of Science and Technology

Nature Communications, 2020, vol. 11, issue 1, 1-15

Abstract: Abstract Magic-sized clusters (MSCs) can be isolated as intermediates in quantum dot (QD) synthesis, and they provide pivotal clues in understanding QD growth mechanisms. We report syntheses for two families of heterogeneous-atom-incorporated InP MSCs that have chlorine or zinc atoms. All the MSCs could be directly synthesized from conventional molecular precursors. Alternatively, each series of MSCs could be prepared by sequential conversions. 386-InP MSCs could be converted to F360-InP:Cl MSCs, then to F399-InP:Cl MSCs. Similarly, F360-InP:Zn MSCs could be converted to F408-InP:Zn MSCs, then to F393-InP:Zn MSCs. As the conversion proceeded, evolution from uni-molecule-like to QD-like characters was observed. Early stage MSCs showed active inter-state conversions in the excited states, which is characteristics of small molecules. Later stage MSCs exhibited narrow photoinduced absorptions at lower-energy region like QDs. The crystal structure also gradually evolved from polytwistane to more zinc-blende.

Date: 2020
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DOI: 10.1038/s41467-020-16855-9

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