Beyond Molecular Conduction: Optical and Thermal Effects in Molecular Junctions

Influence of Coherent Tunneling and Incoherent Hopping on the Charge Transfer Mechanism in Linear Donor–Bridge–Acceptor Systems

“…This was further elaborated by Conwell and co-workers who proposed the polaron-assisted charge transfer mechanism , and used it to explain hole transport in DNA. , The electron-transfer mechanism from tunneling to hopping when increasing bridge length has also been proposed recently by Skourtis and Beratan via the so-called flickering resonance model and applied to charge migration in DNA hairpins. Analytical results for the charge transfer rate have been reported by Segal and Nitzan ,, via the steady-state flux method based on a multihopping model. Other recent simulation studies examine the charge transfer mechanism in DNA − and in other biological systems…”

“…To capture the physics in realistic situations accurately, it is important to account for electron–vibronic interactions. Electron trapping and scattering are also other factors that are known to influence the charge transfer/transport characteristics in realistic systems. − …”

“…Over the years, Marcus theory has been utilized in several studies to describe charge transfer in artificial solar-energy conversion ,, and molecular electronics. ,, The success of this approach relies on a particular electron–vibration interaction, where the initial and final states of the electron transfer process are fully equilibrated polarons localized on different sites, and the transitions between them can be described as a succession of hopping steps . In this manuscript, electron–phonon coupling and polaron theory are used to investigate population localization and delocalization.…”

“…49 This primary vibration can be taken as the effective frequency, together with the effective Huang−Rhys factor 70,71 in a real system with many modes. This model has been utilized to investigate charge transfer, 17,72 exciton dissociation in solar cells, 38 and polaron formation in charge transfer processes. 26 The QME for calculating the density matrix of the primary system, ρ S , is 50,64…”