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; Sungjee Kim

doi:10.1038/s41467-020-16855-9

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, Sungjee Kim

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

20 Citations (Scopus)

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.

Original language	English
Article number	3127
Journal	Nature communications
Volume	11
Issue number	1
DOIs	https://doi.org/10.1038/s41467-020-16855-9
Publication status	Published - 2020 Dec 1

Bibliographical note

Funding Information:
This research at POSTECH was supported by Creative Materials Discovery Program through the National Research Foundation of Korea (NRF) funded by Ministry of Science and ICT (NRF-2019M3D1A1078302) and by NRF grant funded by the Korea government (MSIT) NRF-2019R1A2C2084013. The work at Yonsei University was supported the National Research Foundation of Korea (NRF) grant funded by the Korea government (MEST) (NRF-2016R1E1A1A01943379).

Publisher Copyright:
© 2020, The Author(s).

All Science Journal Classification (ASJC) codes

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
Physics and Astronomy(all)

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10.1038/s41467-020-16855-9

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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.",

author = "Yongju Kwon and Juwon Oh and Eunjae Lee and Lee, {Sang Hyeon} and Anastasia Agnes and Gyuhyun Bang and Jeongmin Kim and Dongho Kim and Sungjee Kim",

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AU - Kim, Dongho

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N2 - 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.

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

Abstract

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