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• W2228393287 endingPage "4897" @default.
• W2228393287 startingPage "4889" @default.
• W2228393287 abstract "The mechanism of charge transfer has been observed to change from tunneling to hopping with increasing numbers of DNA base pairs in polynucleotides and with the length of molecular wires. The aim of this paper is to investigate this transition by examining the population dynamics using a tight-binding Hamiltonian with model parameters to describe a linear donor–bridge–acceptor (D–B–A) system. The model includes a primary vibration and an electron–vibration coupling at each site. A further coupling of the primary vibration with a secondary phonon bath allows the system to dissipate energy to the environment and reach a steady state. We apply the quantum master equation (QME) approach, based on second-order perturbation theory in a quantum dissipative system, to examine the dynamical processes involved in charge-transfer and follow the population transfer rate at the acceptor, ka, to shed light on the transition from tunneling to hopping. With a small tunneling parameter, V, the on-site population tends to localize and form polarons, and the hopping mechanism dominates the transfer process. With increasing V, the population tends to be delocalized and the tunneling mechanism dominates. The competition between incoherent hopping and coherent tunneling governs the mechanism of charge transfer. By varying V and the total number of sites, we also examine the onset of the transition from tunneling to hopping with increasing length." @default.
• W2228393287 created "2016-06-24" @default.
• W2228393287 creator A5026490818 @default.
• W2228393287 creator A5042193329 @default.
• W2228393287 creator A5048985028 @default.
• W2228393287 creator A5062631568 @default.
• W2228393287 creator A5063950840 @default.
• W2228393287 date "2015-11-25" @default.
• W2228393287 modified "2023-10-10" @default.
• W2228393287 title "Influence of Coherent Tunneling and Incoherent Hopping on the Charge Transfer Mechanism in Linear Donor–Bridge–Acceptor Systems" @default.
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• W2228393287 doi "https://doi.org/10.1021/acs.jpclett.5b02154" @default.
• W2228393287 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/26554424" @default.
• W2228393287 hasPublicationYear "2015" @default.
• W2228393287 type Work @default.
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