An effective Hamiltonian approach for Donor-Bridge-Acceptor electronic transitions: Exploring the role of bath memory

Condensed Matter Physics

关键词: super-exchange;    electron transfer theory;    organic photovoltaics;    ultrafast dynamics;    charge transfer;   

DOI  :  10.5488/CMP.19.23803

来源: DOAJ

【 摘 要 】

We present here a formally exact model for electronic transitions between an initial (donor) and final (acceptor) states linked by an intermediate (bridge) state. Our model incorporates a common set of vibrational modes that are coupled to the donor, bridge, and acceptor states and serves as a dissipative bath that destroys quantum coherence between the donor and acceptor. Taking the memory time of the bath as a free parameter, we calculate transition rates for a heuristic 3-state/2 mode Hamiltonian system parameterized to represent the energetics and couplings in a typical organic photovoltaic system. Our results indicate that if the memory time of the bath is of the order of 10-100 fs, a two-state kinetic (i.e., incoherent hopping) model will grossly underestimate overall transition rate.

【 授权许可】

Unknown