Efficient Hole Transfer from CdSe Quantum Dots Enabled by Oxygen-Deficient Polyoxovanadate-Alkoxide Clusters

Cogan, Nicole M. B.; McClelland, Kevin P.; Peter, Chari M.; Rodríguez, Chayan Carmenate; Fertig, Alex A.; Amin, Mitesh; Brennessel, William W.; Krauss, Todd D.; Matson, Ellen M.

doi:10.1021/acs.nanolett.3c02749

Title: Efficient Hole Transfer from CdSe Quantum Dots Enabled by Oxygen-Deficient Polyoxovanadate-Alkoxide Clusters

Journal Article · 07 November 2023 · Nano Letters

DOI: https://doi.org/10.1021/acs.nanolett.3c02749 · OSTI ID:2204920

^[1]; McClelland, Kevin P. ^[1]; Peter, Chari M. ^[1];

^[1]; Fertig, Alex A. ^[1];

^[1];

^[1]

University of Rochester, NY (United States)

A limitation of the implementation of cadmium chalcogenide quantum dots (QDs) in charge transfer systems is the efficient removal of photogenerated holes. Rapid hole transfer has typically required the ex situ functionalization of hole acceptors with groups that can coordinate to the surface of the QD. In addition to being synthetically limiting, this strategy also necessitates a competitive binding equilibrium between the hole acceptor and native, solubilizing ligands on the nanocrystal. Here we show that the incorporation of oxygen vacancies into polyoxovanadate-alkoxide clusters improves hole transfer kinetics by promoting surface interactions between the metal oxide assembly and the QD. Investigating the reactivity of oxygen-deficient clusters with phosphonate-capped QDs reveals reversible complexation of the POValkoxide with a phosphonate ligand at the nanocrystal surface. These findings reveal a new method of facilitating QD–hole acceptor association that bypasses the restrictions of exchange interactions.

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Research Organization:: Univ. of Rochester, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0002106

OSTI ID:: 2204920

Alternate ID(s):: OSTI ID: 2221928

Journal Information:: Nano Letters, Vol. 23, Issue 22; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
colloidal semiconductor nanocrystals
polyoxovanadate clusters
hole transfer
photoluminescence quenching
cadmium selenide
cluster chemistry
ligands
quantum dots
quenching

Title: Efficient Hole Transfer from CdSe Quantum Dots Enabled by Oxygen-Deficient Polyoxovanadate-Alkoxide Clusters

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