Coherent quantum dynamics in donor-bridge-acceptor systems: Beyond the hopping and super-exchange mechanisms

Abstract

The population transfer dynamics of model donor-bridge-acceptor systems is studied by comparing a recently developed polaron-transformed quantum master equation (PQME) with the well-known Redfield and Forster theories of quantum transport. We show that the PQME approach reduces to these two theories in their respective limits of validity and naturally interpolates between them as a function of the system-bath coupling strength. By exploring the parameter space of our model problem, we identify novel regimes of transport dynamics in bridged systems like those encountered in biological and organic energy transfer problems. Furthermore, we demonstrate that three-level systems like the ones studied herein represent ideal minimal models for the identification of quantum coherent transport as embodied in super-exchange phenomena that cannot be captured by Forster-like hopping approaches.

12 pages, 5 figures

References in corpus (5)

• Microscopic theory of singlet exciton fission. II. Application to pentacene dimers and the role of superexchange
• Microscopic theory of singlet exciton fission. I. General formulation
• Correlation-dependent coherent to incoherent transitions in resonant energy transfer dynamics
• Electronic excitation dynamics in multichromophoric systems described via a polaron-representation master equation
• Consistent treatment of coherent and incoherent energy transfer dynamics using a variational master equation

Cited by in corpus (15)

• Delocalized excitons in natural light harvesting complexes
• Spin-selective electron transfer reactions of radical pairs: beyond the Haberkorn master equation
• Coherent dynamics of singlet fission controlled by nonlocal electron-phonon coupling
• Strong system-bath coupling induces negative differential thermal conductance and heat amplification in nonequilibrium two-qubits systems
• Studying rare nonadiabatic dynamics with transition path sampling quantum jump trajectories
• Effects of Donor-Acceptor Quantum Coherence and Non-Markovian Bath on the Distance Dependence of Resonance Energy Transfer
• Modified Fermi's golden rule rate expressions
• Theoretical investigation of non-Förster exciton transfer mechanisms in perylene diimide donor, phenylene bridge, and terrylene diimide acceptor systems
• Ultrafast coherent energy transfer with high efficiency based on plasmonic nanostructures
• Optimal efficiency of quantum transport in a disordered trimer
• No thermalization without correlations
• A polaron theory of quantum thermal transistor in nonequilibrium three-level systems
• Unifying quantum heat transfer and superradiant signature in a nonequilibrium collective-qubit system: a polaron-transformed Redfield approach
• Simple and general unitarity conserving numerical real time propagators of time dependent Schrödinger equation based on Magnus expansion
• Friction as a consistent quantum-mechanical concept