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Förster Resonance Energy Transfer Mapping: A New Methodology to Elucidate Global Structural Features

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Published on: March 16, 2022

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

Shengye Jin¹, Robert C Snoeberger, Abey Issac

¹Department of Chemistry, Emory University, Atlanta, Georgia, USA.

The Journal of Physical Chemistry. B

|March 16, 2010

Summary

Photoinduced electron transfer in sulforhodamine B-based complexes was studied at the single-molecule level. Results reveal fluctuations in electron transfer rates due to molecular conformational changes, impacting fluorescence lifetime.

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High Precision FRET at Single-molecule Level for Biomolecule Structure Determination

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Area of Science:

Photochemistry
Materials Science
Nanotechnology

Background:

Photoinduced interfacial electron transfer (IET) is crucial for energy conversion processes.
Understanding IET at the single-molecule level provides insights into complex interfacial dynamics.
Sulforhodamine B (SRhB) serves as a model fluorophore for studying electron transfer.

Purpose of the Study:

To investigate photoinduced interfacial electron transfer (IET) in SRhB-aminosilane-SnO(2) donor-bridge-acceptor complexes.
To compare IET dynamics on different nanoparticle surfaces (SnO(2) and ZrO(2)).
To explore the heterogeneity and dynamics of IET at the single-molecule level.

Main Methods:

Single-molecule fluorescence spectroscopy to measure fluorescence decays and lifetimes.
Ensemble-averaged fluorescence spectroscopy for comparison.
Computational modeling to understand molecular conformations and electronic coupling.

Main Results:

Single-molecule fluorescence decays align with ensemble averages, indicating comprehensive molecular sampling.
Shorter fluorescence lifetimes were observed on SnO(2) compared to ZrO(2), attributed to IET from SRhB to SnO(2).
Fluctuations in single-molecule lifetimes suggest both static and dynamic heterogeneity in IET.

Conclusions:

The study confirms IET in SRhB-based complexes and highlights differences between SnO(2) and ZrO(2) surfaces.
Observed lifetime fluctuations are linked to dynamic changes in molecular conformation and electronic coupling.
Computational modeling supports the role of conformational dynamics in IET heterogeneity.