Stochastic unraveling of Redfield master equations and its application to electron transfer problems

A method for stochastic unraveling of general time-local quantum masterequations (QMEs) is proposed. The present kind of jump algorithm allows anumerically efficient treatment of QMEs which are not in Lindblad form, i.e.are not positive semidefinite by definition. The unraveling can be achieved byallowing for trajectories with negative weights. Such a property is necessary,e.g. to unravel the Redfield QME and to treat various related problems withhigh numerical efficiency. The method is successfully tested on the dampedharmonic oscillator and on electron transfer models including one and tworeaction coordinates. The obtained results are compared to those from a directpropagation of the reduced density matrix (RDM) as well as from the standardquantum jump method. Comparison of the numerical efficiency is performedconsidering both the population dynamics and the RDM in the Wigner phase spacerepresentation.Comment: accepted in J. Chem. Phys.; 26 pages, 6 figures; the order of authors' names on the title page correcte