Important
Insight into Electron Transfer in Single-Molecule
Junctions Based on Redox Metalloproteins from Transition Voltage Spectroscopy
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Abstract
In a recent experimental work, results
of the first transition
voltage spectroscopy (TVS) investigation on azurin have been reported.
This forms a great case to better understand the electron transfer
through bacterial redox metalloproteins, a process of fundamental
importance from chemical, physical, and biological perspectives, and
of practical importance for nano(bio)electronics. In the present paper
we challenge the tentative interpretation put forward in the aforementioned
experimental study and propose a different theoretical interpretation.
To explain the experimental TVS data, we adopt an extended Newns–Anderson
framework, whose accuracy and robustness is demonstrated. We show
that that this framework clearly meets the need to obtain a consistent
description across experiments. Most importantly, the presently proposed
theoretical approach permits unraveling novel aspects on the impact
of the electrochemical scanning microscope environment on the charge
transport through single-(bio)molecule junctions based on redox units.
The usefulness of TVS as a versatile method of investigation, also
able to provide important insight into the charge transport through
metalloproteins, is emphasized