ArticleProceedings of the National Academy of Sciences of the United States of America2014
Biological charge transfer via flickering resonance.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2014. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 51 papers.
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51 citing papers in PubMed, 167 citations in OpenAlex.
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- New Perspective on Electron Transfer through Molecules.The journal of physical chemistry letters · 2022Article
- Modeling Charge Transfer Reactions by Hopping between Electronic Ground State Minima: Application to Hole Transfer between DNA Bases.Molecules (Basel, Switzerland) · 2022Article
- Molecular Wires for Efficient Long-Distance Triplet Energy Transfer.The journal of physical chemistry letters · 2022Article
- Electron Transfer Rates in Polar and Non-Polar Environments: a Generalization of Marcus' Theory to Include an Effective Treatment of Tunneling Effects.The journal of physical chemistry letters · 2022Article
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- Generalization on Entropy-Ruled Charge and Energy Transport for Organic Solids and Biomolecular Aggregates.ACS omega · 2022Article
- The Time Scale of Electronic Resonance in Oxidized DNA as Modulated by Solvent Response: An MD/QM-MM Study.Molecules (Basel, Switzerland) · 2021Article
- DNA Electrochemistry: Charge-Transport Pathways through DNA Films on Gold.Journal of the American Chemical Society · 2021Article
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Authors and funding
5 authors at 2 institutions in 2 countries.
Funding
No grant is acknowledged in the PubMed record.
Abstract
Biological electron-transfer (ET) reactions are typically described in the framework of coherent two-state electron tunneling or multistep hopping. However, these ET reactions may involve multiple redox cofactors in van der Waals contact with each other and with vibronic broadenings on the same scale as the energy gaps among the species. In this regime, fluctuations of the molecular structures and of the medium can produce transient energy level matching among multiple electronic states. This transient degeneracy, or flickering electronic resonance among states, is found to support coherent (ballistic) charge transfer. Importantly, ET rates arising from a flickering resonance (FR) mechanism will decay exponentially with distance because the probability of energy matching multiple states is multiplicative. The distance dependence of FR transport thus mimics the exponential decay that is usually associated with electron tunneling, although FR transport involves real carrier population on the bridge and is not a tunneling phenomenon. Likely candidates for FR transport are macromolecules with ET groups in van der Waals contact: DNA, bacterial nanowires, multiheme proteins, strongly coupled porphyrin arrays, and proteins with closely packed redox-active residues. The theory developed here is used to analyze DNA charge-transfer kinetics, and we find that charge-transfer distances up to three to four bases may be accounted for with this mechanism. Thus, the observed rapid (exponential) distance dependence of DNA ET rates over distances of ≲ 15 Å does not necessarily prove a tunneling mechanism.
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