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arXiv:1612.00213 · Infinite Dimensional Analysis Quantum Probability and Related Topics

Flows in non-equilibrium quantum systems and quantum photosynthesis

S. V. Kozyrev, A. A. Mironov, Alexander Evgen’evich Teretenkov, I. V. Volovich

Published Dec 1, 2017• 21 citations
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Abstract

A three-level quantum system interacting with non-equilibrium environment is investigated. The stationary state of the system is found (both for non-coherent and coherent environment) and relaxation and decoherence to the stationary state is described. The stationary state of the system will be non-equilibrium and will generate flows. We describe the dependence of the flows on the state of the environment. We also discuss application of this model to the problem of quantum photosynthesis, in particular, to the description of flows of excitons and generation of excitonic coherences.

DOI
10.1142/s0219025717500217

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A three-level quantum system interacting with non-equilibrium environment is investigated. The stationary state of the system is found (both for non-coherent and coherent environment) and relaxation and decoherence to the stationary state is described. The stationary state of the system will be non-equilibrium and will generate flows. We describe the dependence of the flows on the state of the environment. We also discuss application of this model to the problem of quantum photosynthesis, in particular, to the description of flows of excitons and generation of excitonic coherences.
The mechanism of vibronic amplification of transport of excitons has been discussed in connection with quantum photosynthesis. Vibrons (some modes of vibrations of molecules) have been observed experimentally in photosynthetic systems. In the present paper we consider models of vibronic amplification of quantum transfer in which the generation of vibrons as a coherent vibrational mode is described by an analog of the semiclassical laser theory. We study two models: a model of nonequilibrium three-level system with vibronic mode, and a variant of a model of lasing without inversion. We conjecture that the dark states discussed in connection with quantum photosynthesis might be related to the mechanism of vibronic “laser” without inversion, which amplifies the transfer of excitons. We prove that in the presence of a vibronic mode the transfer rate of excitons increases, and compute the dependence of the transfer rate on the parameters of the model.
Transport in nonequilibrium degenerate quantum systems is investigated. The transfer rate depends on the parameters of the system. In this paper we investigate the dependence of the flow (transfer rate) on the angle between “bright” vectors (which define the interaction of the system with the environment). We show that in some approximation for the system under investigation the flow is proportional to the cosine squared of the angle between the “bright” vectors. Earlier the author has shown that in this degenerate quantum system excitation of nondecaying quantum “dark” states is possible; moreover, the effectiveness of this process is proportional to the sine squared of the angle between the “bright” vectors (this phenomenon was discussed as a possible model of excitation of quantum coherence in quantum photosynthesis). Thus quantum transport and excitation of dark states are competing processes; “dark” states can be considered as a result of leakage of quantum states in a quantum thermodynamic machine which performs the quantum transport.
Abstract Thermodynamic irreversibility is well characterized by the entropy production arising from non-equilibrium quantum processes. We show that the entropy production of a quantum system undergoing open-system dynamics can be formally split into a term that only depends on population unbalances, and one that is underpinned by quantum coherences. This allows us to identify a genuine quantum contribution to the entropy production in non-equilibrium quantum processes. We discuss how these features emerge both in Lindblad-Davies differential maps and finite maps subject to the constraints of thermal operations. We also show how this separation naturally leads to two independent entropic conservation laws for the global system-environment dynamics, one referring to the redistribution of populations between system and environment and the other describing how the coherence initially present in the system is distributed into local coherences in the environment and non-local coherences in the system-environment state. Finally, we discuss how the processing of quantum coherences and the incompatibility of non-commuting measurements leads to fundamental limitations in the description of quantum trajectories and fluctuation theorems.
Interaction between a quantum system and its environment can induce stationary coherences---off-diagonal elements in the reduced system density matrix in the energy eigenstate basis---even at equilibrium. This work investigates the ``quantumness'' of such phenomena by examining the ability of classical and semiclassical models to describe equilibrium stationary coherence in the multilevel spin boson model, a common model for light-harvesting systems. A well justified classical harmonic-oscillator model is found to fail to capture equilibrium coherence. This failure is attributed to the effective weakness of classical system-bath interactions due to the absence of a discrete system energy spectrum and, consequently, of quantized shifts in oscillator coordinates. Semiclassical coherences also vanish for a dimeric model with parameters typical of biological light harvesting, i.e., where both system sites couple to the bath with the same reorganization energy. In contrast, equilibrium coherence persists in a fully quantum description of the same system, suggesting a uniquely quantum-mechanical origin for equilibrium stationary coherence in, e.g., photosynthetic systems. Finally, as a computational tool, a perturbative expansion is introduced that, at third order in $\ensuremath{\hbar}$, gives qualitatively correct behavior at ambient temperatures for all configurations examined.
In this paper, we present a theoretical description to the quantum coherence and decoherence phenomena of energy transfer in photosynthesis observed in a recent experiment [see Science 316, 1462 (2007)]. As a successive two-color laser pulses with selected frequencies cast on a sample of the photosynthetic purple bacterium Rb. sphaeroides two resonant excitations of electrons in chromophores can be generated. However, this effective two-level subsystem will interact with its protein environment and decoherence is inevitable. We describe this subsystem coupled with its environment as a dynamical spin-boson model. The non-Markovian decoherence dynamics is described using a quasi-adiabatic propagator path integral (QUAPI) approach. With the photon-induced effective time-dependent level splitting energy and level flip coupling coefficient between the two excited states and the environment-induced non-Markovian decoherence dynamics, our theoretical result is in good agreement with the experimental data.
Analyzing the dynamics of open quantum systems has a long history in mathematics and physics. Depending on the system at hand, basic physical phenomena that one would like to explain are, for example, convergence to equilibrium, the dynamics of quantum coherences (decoherence) and quantum correlations (entanglement), or the emergence of heat and particle fluxes in non-equilibrium situations. From the mathematical physics perspective, one of the main challenges is to derive the irreversible dynamics of the open system, starting from a unitary dynamics of the system and its environment. The repeated interactions systems considered in these notes are models of non-equilibrium quantum statistical mechanics. They are relevant in quantum optics, and more generally, serve as a relatively well treatable approximation of a more difficult quantum dynamics. In particular, the repeated interaction models allow to determine the large time (stationary) asymptotics of quantum systems out of equilibrium.