Surface-Area-Dependent Electron Transfer between Isoenergetic 2D Quantum Wells and a Molecular Acceptor

Benjamin T. Diroll; Igor Fedin; Pierre Darancet; Dmitri V. Talapin; Richard D. Schaller

doi:10.1021/jacs.6b06572

Surface-Area-Dependent Electron Transfer between Isoenergetic 2D Quantum Wells and a Molecular Acceptor

Benjamin T. Diroll, Igor Fedin, Pierre Darancet, Dmitri V. Talapin, Richard D. Schaller^*

^*Corresponding author for this work

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

36 Scopus citations

Abstract

We report measurements of electron transfer rates for four isoenergetic donor-acceptor pairs comprising a molecular electron acceptor, methylviologen (MV), and morphology-controlled colloidal semiconductor nanoparticles of CdSe. The four nanoparticles include a spherical quantum dot (QD) and three differing lateral areas of 4-monolayer-thick nanoplatelets (NPLs), each with a 2.42 eV energy gap. As such, the measurements, performed via ultrafast photoluminescence, relate the dependence of charge transfer rate on the spatial extent of the initial electron-hole pair wave function explicitly, which we show for the first time to be related to surface area in this regime that is intermediate between homogeneous and heterogeneous charge transfer as well as 2D to 0D electron transfer. The observed nonlinear dependence of rate with surface area is attributed to exciton delocalization within each structure, which we show via temperature-dependent absorption measurements remains constant.

Original language	English (US)
Pages (from-to)	11109-11112
Number of pages	4
Journal	Journal of the American Chemical Society
Volume	138
Issue number	35
DOIs	https://doi.org/10.1021/jacs.6b06572
State	Published - Sep 7 2016

Funding

This work was performed in part at the Center for Nanoscale Materials, a US Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility under Contract No. DEAC02- 06CH11357.

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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title = "Surface-Area-Dependent Electron Transfer between Isoenergetic 2D Quantum Wells and a Molecular Acceptor",

abstract = "We report measurements of electron transfer rates for four isoenergetic donor-acceptor pairs comprising a molecular electron acceptor, methylviologen (MV), and morphology-controlled colloidal semiconductor nanoparticles of CdSe. The four nanoparticles include a spherical quantum dot (QD) and three differing lateral areas of 4-monolayer-thick nanoplatelets (NPLs), each with a 2.42 eV energy gap. As such, the measurements, performed via ultrafast photoluminescence, relate the dependence of charge transfer rate on the spatial extent of the initial electron-hole pair wave function explicitly, which we show for the first time to be related to surface area in this regime that is intermediate between homogeneous and heterogeneous charge transfer as well as 2D to 0D electron transfer. The observed nonlinear dependence of rate with surface area is attributed to exciton delocalization within each structure, which we show via temperature-dependent absorption measurements remains constant.",

author = "Diroll, \{Benjamin T.\} and Igor Fedin and Pierre Darancet and Talapin, \{Dmitri V.\} and Schaller, \{Richard D.\}",

note = "Funding Information: This work was performed in part at the Center for Nanoscale Materials, a US Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility under Contract No. DEAC02- 06CH11357. Publisher Copyright: {\textcopyright} 2016 American Chemical Society.",

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AU - Diroll, Benjamin T.

AU - Fedin, Igor

AU - Darancet, Pierre

AU - Talapin, Dmitri V.

AU - Schaller, Richard D.

N1 - Funding Information: This work was performed in part at the Center for Nanoscale Materials, a US Department of Energy, Office of Science, Office of Basic Energy Sciences User Facility under Contract No. DEAC02- 06CH11357. Publisher Copyright: © 2016 American Chemical Society.

PY - 2016/9/7

Y1 - 2016/9/7

N2 - We report measurements of electron transfer rates for four isoenergetic donor-acceptor pairs comprising a molecular electron acceptor, methylviologen (MV), and morphology-controlled colloidal semiconductor nanoparticles of CdSe. The four nanoparticles include a spherical quantum dot (QD) and three differing lateral areas of 4-monolayer-thick nanoplatelets (NPLs), each with a 2.42 eV energy gap. As such, the measurements, performed via ultrafast photoluminescence, relate the dependence of charge transfer rate on the spatial extent of the initial electron-hole pair wave function explicitly, which we show for the first time to be related to surface area in this regime that is intermediate between homogeneous and heterogeneous charge transfer as well as 2D to 0D electron transfer. The observed nonlinear dependence of rate with surface area is attributed to exciton delocalization within each structure, which we show via temperature-dependent absorption measurements remains constant.

AB - We report measurements of electron transfer rates for four isoenergetic donor-acceptor pairs comprising a molecular electron acceptor, methylviologen (MV), and morphology-controlled colloidal semiconductor nanoparticles of CdSe. The four nanoparticles include a spherical quantum dot (QD) and three differing lateral areas of 4-monolayer-thick nanoplatelets (NPLs), each with a 2.42 eV energy gap. As such, the measurements, performed via ultrafast photoluminescence, relate the dependence of charge transfer rate on the spatial extent of the initial electron-hole pair wave function explicitly, which we show for the first time to be related to surface area in this regime that is intermediate between homogeneous and heterogeneous charge transfer as well as 2D to 0D electron transfer. The observed nonlinear dependence of rate with surface area is attributed to exciton delocalization within each structure, which we show via temperature-dependent absorption measurements remains constant.

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Surface-Area-Dependent Electron Transfer between Isoenergetic 2D Quantum Wells and a Molecular Acceptor

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