Abstract
We present a non-Markovian quantum jump (NMQJ) approach for simulating coherent energy transfer dynamics in molecular systems in the presence of laser fields. By combining a coherent modified Redfield theory (CMRT) and a NMQJ method, this new approach inherits the broad-range validity from the CMRT and highly efficient propagation from the NMQJ. To implement NMQJ propagation of CMRT, we show that the CMRT master equation can be cast into a generalized Lindblad form. Moreover, we extend the NMQJ approach to treat time-dependent Hamiltonian, enabling the description of excitonic systems under coherent laser fields. As a benchmark of the validity of this new method, we show that the CMRT–NMQJ method accurately describes the energy transfer dynamics in a prototypical photosynthetic complex. Finally, we apply this new approach to simulate the quantum dynamics of a dimer system coherently excited to coupled single-excitation states under the influence of laser fields, which allows us to investigate the interplay between the photoexcitation process and ultrafast energy transfer dynamics in the system. We demonstrate that laser-field parameters significantly affect coherence dynamics of photoexcitations in excitonic systems, which indicates that the photoexcitation process must be explicitly considered in order to properly describe photon-induced dynamics in photosynthetic systems. This work should provide a valuable tool for efficient simulations of coherent control of energy flow in photosynthetic systems and artificial optoelectronic materials.
Highlights
During the past decade, much progress has been achieved in both experimental and theoretical explorations of photosynthetic excitation energy transfer (EET), e.g. EET pathways determined by pump-probe as well as two-dimensional (2D) electronic spectroscopy (2DES) [1,2,3], coherent EET dynamics revealed by 2DES [4,5,6], and theoretical studies to elucidate mechanisms of EET [7,8,9,10]
In order to make the coherent modified Redfield theory (CMRT) suitable for time-propagation by the non-Markovian quantum jump (NMQJ) method, we show that the CMRT quantum master equation can be rewritten in a generalized Lindblad form
These new developments allow the efficient calculation of quantum dynamics of photosynthetic complexes in the presence of laser fields
Summary
Much progress has been achieved in both experimental and theoretical explorations of photosynthetic excitation energy transfer (EET), e.g. EET pathways determined by pump-probe as well as two-dimensional (2D) electronic spectroscopy (2DES) [1,2,3], coherent EET dynamics revealed by 2DES [4,5,6], and theoretical studies to elucidate mechanisms of EET [7,8,9,10]. An accurate yet numerically efficient method for simulating quantum dynamics in photosynthetic systems in the presence of coherent laser fields is highly desirable. We combine a coherent modified Redfield theory (CMRT) [30] and a nonMarkovian quantum jump (NMQJ) method [31,32,33] to develop an efficient approach for coherent EET dynamics in photosynthetic systems under the influence of light–matter interactions. As a generalization of the modified Redfield theory, the CMRT approach provides a complete description of quantum dynamics of the systems density matrix. To make use of the NMQJ method, which has been shown to be efficient for simulating quantum dynamics in EET [33, 42], we recast the CMRT equation into a generalized Lindblad form [43]. The details in the derivation and validity of the CMRT approach is outside the scope of this paper and will be published elsewhere [30]
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