Consistent treatment of coherent and incoherent energy transfer dynamics using a variational master equation.
نویسندگان
چکیده
We investigate the energy transfer dynamics in a donor-acceptor model by developing a time-local master equation technique based on a variational transformation of the underlying Hamiltonian. The variational transformation allows a minimisation of the Hamiltonian perturbation term dependent on the system parameters, and consequently results in a versatile master equation valid over a range of system-bath coupling strengths, temperatures, and environmental spectral densities. While our formalism reduces to the well-known Redfield, Förster and polaron forms in the appropriate limits, in general it is not equivalent to perturbing in either the system-environment or donor-acceptor coupling strengths, and hence can provide reliable results between these limits as well. Moreover, we show how to include the effects of both environmental correlations and non-equilibrium preparations within the formalism.
منابع مشابه
A multi-site variational master equation approach to dissipative energy transfer
Unitary transformations can allow one to study open quantum systems in situations for which standard, weak-coupling type approximations are not valid. We develop here an extension of the variational (polaron) transformation approach to open system dynamics, which applies to arbitrarily large exciton transport networks with local environments. After deriving a time-local master equation in the t...
متن کاملTheoretical Advances toward Understanding Recent Experiments in Biophysical Chemistry
Several theoretical advances are presented, with the common theme of helping better understand and guide recent experiments in biophysical chemistry. In Chapter 2, I consider a recent criticism of the Jarzynski equality, notably that a breakdown in the connection between work and changes in the Hamiltonian for time-dependent systems causes the Jarzynski equality to produce unphysical results. I...
متن کاملUnified treatment of quantum coherent and incoherent hopping dynamics in electronic energy transfer: reduced hierarchy equation approach.
A new quantum dynamic equation for excitation energy transfer is developed which can describe quantum coherent wavelike motion and incoherent hopping in a unified manner. The developed equation reduces to the conventional Redfield theory and Forster theory in their respective limits of validity. In the regime of coherent wavelike motion, the equation predicts several times longer lifetime of el...
متن کاملCoherent versus incoherent excitation energy transfer in molecular systems.
We investigate the Markovian limit of a polaronic quantum master equation for coherent resonance energy transfer proposed recently by Jang et al. [J. Chem. Phys. 129, 101104 (2008)]. An expression for the rate of excitation energy transfer (EET) is derived and shown to exhibit both coherent and incoherent contributions. We then apply this theory to calculated EET rates for model dimer systems, ...
متن کاملTHE SPINLESS SALPETER EQUATION AND MESON DYNAMICS
Applying the variational method, the spinless reduced Bethe-Salpeter (RBS) equation is solved for the mesonic systems, and the mass spectra are obtained. The method is applied to the Hamiltonian with the Gaussian and hydrogen-type trial wave functions, and different potential models are examined. The results for the different potentials are in challenge in light mesons, while they are consisten...
متن کاملذخیره در منابع من
با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید
عنوان ژورنال:
- The Journal of chemical physics
دوره 135 11 شماره
صفحات -
تاریخ انتشار 2011