Subpicosecond Photoinduced Hole Transfer from a CdS Quantum Dot to a Molecular Acceptor Bound Through an Exciton-Delocalizing Ligand

Shichen Lian; David J. Weinberg; Rachel D. Harris; Mohamad S. Kodaimati; Emily A Weiss

doi:10.1021/acsnano.6b02814

Subpicosecond Photoinduced Hole Transfer from a CdS Quantum Dot to a Molecular Acceptor Bound Through an Exciton-Delocalizing Ligand

Shichen Lian, David J. Weinberg, Rachel D. Harris, Mohamad S. Kodaimati, Emily A Weiss

Northwestern University

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

50 Citations (Scopus)

Abstract

This paper describes the enhancement of the rate of hole transfer from a photoexcited CdS quantum dot (QD), with radius R = 2.0 nm, to a molecular acceptor, phenothiazine (PTZ), by linking the donor and acceptor through a phenyldithiocarbamate (PTC) linker, which is known to lower the confinement energy of the excitonic hole. Upon adsorption of PTC, the bandgap of the QD decreases due to delocalization of the exciton, primarily the excitonic hole, into interfacial states of mixed QD/PTC character. This delocalization enables hole transfer from the QD to PTZ in 1H NMR. This work provides direct spectroscopic evidence of the enhancement of the rate of hole extraction from a colloidal QD through covalent linkage of a hole acceptor through an exciton-delocalizing ligand.

Original language	English
Pages (from-to)	6372-6382
Number of pages	11
Journal	ACS Nano
Volume	10
Issue number	6
DOIs	https://doi.org/10.1021/acsnano.6b02814
Publication status	Published - Jun 28 2016

Keywords

CdS quantum dot
dithiocarbamate
electronic coupling
exciton delocalization
hole transfer
transient absorption spectroscopy

ASJC Scopus subject areas

Engineering(all)
Materials Science(all)
Physics and Astronomy(all)

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title = "Subpicosecond Photoinduced Hole Transfer from a CdS Quantum Dot to a Molecular Acceptor Bound Through an Exciton-Delocalizing Ligand",

abstract = "This paper describes the enhancement of the rate of hole transfer from a photoexcited CdS quantum dot (QD), with radius R = 2.0 nm, to a molecular acceptor, phenothiazine (PTZ), by linking the donor and acceptor through a phenyldithiocarbamate (PTC) linker, which is known to lower the confinement energy of the excitonic hole. Upon adsorption of PTC, the bandgap of the QD decreases due to delocalization of the exciton, primarily the excitonic hole, into interfacial states of mixed QD/PTC character. This delocalization enables hole transfer from the QD to PTZ in 1H NMR. This work provides direct spectroscopic evidence of the enhancement of the rate of hole extraction from a colloidal QD through covalent linkage of a hole acceptor through an exciton-delocalizing ligand.",

keywords = "CdS quantum dot, dithiocarbamate, electronic coupling, exciton delocalization, hole transfer, transient absorption spectroscopy",

author = "Shichen Lian and Weinberg, {David J.} and Harris, {Rachel D.} and Kodaimati, {Mohamad S.} and Weiss, {Emily A}",

year = "2016",

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language = "English",

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AU - Lian, Shichen

AU - Weinberg, David J.

AU - Harris, Rachel D.

AU - Kodaimati, Mohamad S.

AU - Weiss, Emily A

PY - 2016/6/28

Y1 - 2016/6/28

N2 - This paper describes the enhancement of the rate of hole transfer from a photoexcited CdS quantum dot (QD), with radius R = 2.0 nm, to a molecular acceptor, phenothiazine (PTZ), by linking the donor and acceptor through a phenyldithiocarbamate (PTC) linker, which is known to lower the confinement energy of the excitonic hole. Upon adsorption of PTC, the bandgap of the QD decreases due to delocalization of the exciton, primarily the excitonic hole, into interfacial states of mixed QD/PTC character. This delocalization enables hole transfer from the QD to PTZ in 1H NMR. This work provides direct spectroscopic evidence of the enhancement of the rate of hole extraction from a colloidal QD through covalent linkage of a hole acceptor through an exciton-delocalizing ligand.

AB - This paper describes the enhancement of the rate of hole transfer from a photoexcited CdS quantum dot (QD), with radius R = 2.0 nm, to a molecular acceptor, phenothiazine (PTZ), by linking the donor and acceptor through a phenyldithiocarbamate (PTC) linker, which is known to lower the confinement energy of the excitonic hole. Upon adsorption of PTC, the bandgap of the QD decreases due to delocalization of the exciton, primarily the excitonic hole, into interfacial states of mixed QD/PTC character. This delocalization enables hole transfer from the QD to PTZ in 1H NMR. This work provides direct spectroscopic evidence of the enhancement of the rate of hole extraction from a colloidal QD through covalent linkage of a hole acceptor through an exciton-delocalizing ligand.

KW - CdS quantum dot

KW - dithiocarbamate

KW - electronic coupling

KW - exciton delocalization

KW - hole transfer

KW - transient absorption spectroscopy

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