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Colloidal CdSe nanocrystals are inherently defective.

ABSTRACT: 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.

SUBMITTER: Goldzak T

PROVIDER: S-EPMC7873310 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Colloidal CdSe nanocrystals are inherently defective.

Goldzak Tamar T McIsaac Alexandra R AR Van Voorhis Troy T

Nature communications 20210209 1

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 ...[more]

PMID: 33563985

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