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Formulation of Long-Range Transport Rates through Molecular Bridges: From Unfurling to Hopping.
- Source :
-
The journal of physical chemistry letters [J Phys Chem Lett] 2018 Aug 02; Vol. 9 (15), pp. 4139-4145. Date of Electronic Publication: 2018 Jul 12. - Publication Year :
- 2018
-
Abstract
- Weak fluctuations about the rigid equilibrium structure of ordered molecular bridges drive charge transfer in donor-bridge-acceptor systems via quantum unfurling, which differs from both hopping and ballistic transfer, yet static disorder (low frequency motions) in the bridge is shown to induce a change of mechanism from unfurling to hopping when local fluctuations along the molecular bridge are uncorrelated. Remarkably, these two different transport mechanisms manifest in similar charge-transfer rates, which are nearly independent of the molecular bridge length. We propose an experimental test for distinguishing unfurling from hopping in DNA models with different helix directionality. A unified formulation explains the apparent similarity in the length dependence of the transfer rate despite the difference in the underlying transport mechanisms.
Details
- Language :
- English
- ISSN :
- 1948-7185
- Volume :
- 9
- Issue :
- 15
- Database :
- MEDLINE
- Journal :
- The journal of physical chemistry letters
- Publication Type :
- Academic Journal
- Accession number :
- 29961322
- Full Text :
- https://doi.org/10.1021/acs.jpclett.8b01581