Colloidal CdSe nanocrystals are inherently defective
Name
s41467-021-21153-z.pdf
Description
Published version
Size
1.23 MB
Format
Adobe PDF
Checksum (MD5)
3233c57d3d62869d35c2103f134bf7ea
Author(s)
Goldzak, Tamar
McIsaac, Alexandra R
Van Voorhis, Troy
Date Issued
2021
Journal
Nature Communications
Publisher
Springer Science and Business Media LLC
Citation
Goldzak, Tamar, McIsaac, Alexandra R and Van Voorhis, Troy. 2021. "Colloidal CdSe nanocrystals are inherently defective." Nature Communications, 12 (1).
Version
Final published version
Abstract
© 2021, The Author(s). Colloidal CdSe nanocrystals (NCs) have shown promise in applications ranging from LED displays to medical imaging. Their unique photophysics depend sensitively on the presence or absence of surface defects. Using simulations, we show that CdSe NCs are inherently defective; even for stoichiometric NCs with perfect ligand passivation and no vacancies or defects, we still observe that the low energy spectrum is dominated by dark, surface-associated excitations, which are more numerous in larger NCs. Surface structure analysis shows that the majority of these states involve holes that are localized on two-coordinate Se atoms. As chalcogenide atoms are not passivated by any Lewis base ligand, varying the ligand should not dramatically change the number of dark states, which we confirm by simulating three passivation schemes. Our results have significant implications for understanding CdSe NC photophysics, and suggest that photochemistry and short-range photoinduced charge transfer should be much more facile than previously anticipated.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
Terms of Use
Creative Commons Attribution 4.0 International license
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DOI of Published Version
https://doi.org/10.1038/S41467-021-21153-Z
