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تسجيل مستخدم جديدCoherent and incoherent theories for photosynthetic energy transfer
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There is a remarkable characteristic of photosynthesis in nature, that is, the energy transfer efficiency is close to 100%. Recently, due to the rapid progress made in the experimental techniques, quantum coherent effects have been experimentally demonstrated. Traditionally, the incoherent theories are capable of calculating the energy transfer efficiency, e.g., (generalized) Forster theory and modified Redfield theory. However, in order to describe the quantum coherent effects in photosynthesis, the coherent theories have been developed, such as hierarchical equation of motion, quantum path integral, coherent modified Redfield theory, small-polaron quantum master equation, and general Bloch-Redfield theory in addition to the Redfield theory. Here, we summarize the main points of the above approaches, which might be beneficial to the quantum simulation of quantum dynamics of exciton energy transfer in natural photosynthesis, and shed light on the design of artificial light-harvesting devices.
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Giant strides in ultrashort laser pulse technology have enabled real-time observation of dynamical processes in complex molecular systems. Specifically, the discovery of oscillatory transients in the two-dimensional electronic spectra of photosynthet
ic systems stimulated a number of theoretical investigations exploring possible physical mechanisms of the remarkable quantum efficiency of light harvesting processes. However, the theories employed have reached a high degree of sophistication and have become complex, making it difficult to gain insights into microscopic processes and biologically significant questions. In this work, we revisit the elementary aspects of environment-induced fluctuations in the involved electronic energies and present a simple way to understand energy flow with the intuitive picture of relaxation in a funnel-type free-energy landscape. The presented free-energy description of energy transfer reveals that typical photosynthetic systems operate in an almost barrierless regime. The approach also provides insights into the distinction between coherent and incoherent energy transfer and criteria by which the necessity of the vibrational assistance is considered.
We present a non-Markovian quantum jump 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 non-Markovian quantum jump (NMQJ) me
thod, 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 casted 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.
Near-unity energy transfer efficiency has been widely observed in natural photosynthetic complexes. This phenomenon has attracted broad interest from different fields, such as physics, biology, chemistry and material science, as it may offer valuable
insights into efficient solar-energy harvesting. Recently, quantum coherent effects have been discovered in photosynthetic light harvesting, and their potential role on energy transfer has seen heated debate. Here, we perform an experimental quantum simulation of photosynthetic energy transfer using nuclear magnetic resonance (NMR). We show that an N- chromophore photosynthetic complex, with arbitrary structure and bath spectral density, can be effectively simulated by a system with log2 N qubits. The computational cost of simulating such a system with a theoretical tool, like the hierarchical equation of motion, which is exponential in N, can be potentially reduced to requiring a just polynomial number of qubits N using NMR quantum simulation. The benefits of performing such quantum simulation in NMR are even greater when the spectral density is complex, as in natural photosynthetic complexes. These findings may shed light on quantum coherence in energy transfer and help to provide design principles for efficient artificial light harvesting.
The non-equilibrium stationary coherences that form in donor-acceptor systems are investigated to determine their relationship to the efficiency of energy transfer to a neighboring reaction center. It is found that the effects of asymmetry in the dim
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