Single-molecule interfacial electron transfer in donor-bridge-nanoparticle acceptor complexes

Shengye Jin; Robert C. Snoeberger; Abey Issac; David Stockwell; Victor S. Batista; Tianquan Lian

doi:10.1021/jp911662g

Single-molecule interfacial electron transfer in donor-bridge-nanoparticle acceptor complexes

Shengye Jin, Robert C. Snoeberger, Abey Issac, David Stockwell, Victor S. Batista, Tianquan Lian^*

^*Corresponding author for this work

Physics

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

22 Citations (Scopus)

Abstract

Photoinduced interfacial electron transfer (IET) in sulforhodamine B (SRhB)-aminosilane-Tin oxide (SnO₂) nanoparticle donor-bridge- acceptor complexes has been studied on a single molecule and ensemble average level. On both SnO₂ and ZrO₂, the sum of single molecule fluorescence decays agree with the ensemble average results, suggesting complete sampling of molecules under single molecule conditions. Shorter fluorescence lifetime on SnO₂ than on ZrO₂ is observed and attributed to IET from SRhB to SnO₂. Single molecule lifetimes fluctuate with time and vary among different molecules, suggesting both static and dynamic IET heterogeneity in this system. Computational modeling of the complexes shows a distribution of molecular conformation, leading to a distribution of electronic coupling strengths and ET rates. It is likely that the conversion between these conformations led to the fluctuation of ET rate and fluorescence lifetime on the single molecule level.

Original language	English
Pages (from-to)	14309-14319
Number of pages	11
Journal	Journal of Physical Chemistry B
Volume	114
Issue number	45
DOIs	https://doi.org/10.1021/jp911662g
Publication status	Published - Dec 8 2010

ASJC Scopus subject areas

Physical and Theoretical Chemistry
Materials Chemistry
Surfaces, Coatings and Films

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abstract = "Photoinduced interfacial electron transfer (IET) in sulforhodamine B (SRhB)-aminosilane-Tin oxide (SnO2) nanoparticle donor-bridge- acceptor complexes has been studied on a single molecule and ensemble average level. On both SnO2 and ZrO2, the sum of single molecule fluorescence decays agree with the ensemble average results, suggesting complete sampling of molecules under single molecule conditions. Shorter fluorescence lifetime on SnO2 than on ZrO2 is observed and attributed to IET from SRhB to SnO2. Single molecule lifetimes fluctuate with time and vary among different molecules, suggesting both static and dynamic IET heterogeneity in this system. Computational modeling of the complexes shows a distribution of molecular conformation, leading to a distribution of electronic coupling strengths and ET rates. It is likely that the conversion between these conformations led to the fluctuation of ET rate and fluorescence lifetime on the single molecule level.",

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AU - Jin, Shengye

AU - Snoeberger, Robert C.

AU - Issac, Abey

AU - Stockwell, David

AU - Batista, Victor S.

AU - Lian, Tianquan

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N2 - Photoinduced interfacial electron transfer (IET) in sulforhodamine B (SRhB)-aminosilane-Tin oxide (SnO2) nanoparticle donor-bridge- acceptor complexes has been studied on a single molecule and ensemble average level. On both SnO2 and ZrO2, the sum of single molecule fluorescence decays agree with the ensemble average results, suggesting complete sampling of molecules under single molecule conditions. Shorter fluorescence lifetime on SnO2 than on ZrO2 is observed and attributed to IET from SRhB to SnO2. Single molecule lifetimes fluctuate with time and vary among different molecules, suggesting both static and dynamic IET heterogeneity in this system. Computational modeling of the complexes shows a distribution of molecular conformation, leading to a distribution of electronic coupling strengths and ET rates. It is likely that the conversion between these conformations led to the fluctuation of ET rate and fluorescence lifetime on the single molecule level.

AB - Photoinduced interfacial electron transfer (IET) in sulforhodamine B (SRhB)-aminosilane-Tin oxide (SnO2) nanoparticle donor-bridge- acceptor complexes has been studied on a single molecule and ensemble average level. On both SnO2 and ZrO2, the sum of single molecule fluorescence decays agree with the ensemble average results, suggesting complete sampling of molecules under single molecule conditions. Shorter fluorescence lifetime on SnO2 than on ZrO2 is observed and attributed to IET from SRhB to SnO2. Single molecule lifetimes fluctuate with time and vary among different molecules, suggesting both static and dynamic IET heterogeneity in this system. Computational modeling of the complexes shows a distribution of molecular conformation, leading to a distribution of electronic coupling strengths and ET rates. It is likely that the conversion between these conformations led to the fluctuation of ET rate and fluorescence lifetime on the single molecule level.

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