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Register a new userEffects of system-bath entanglement on the performance of light-harvesting systems: A quantum heat engine perspective
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We explore energy transfer in a generic three-level system, which is coupled to three non-equilibrium baths. Built on the concept of quantum heat engine, our three-level model describes non-equilibrium quantum processes including light-harvesting energy transfer, nano-scale heat transfer, photo-induced isomerization, and photovoltaics in double quantum-dots. In the context of light-harvesting, the excitation energy is first pumped up by sunlight, then is transferred via two excited states which are coupled to a phonon bath, and finally decays to the ground state. The efficiency of this process is evaluated by steady state analysis via a polaron-transformed master equation; thus a wide range of the system-phonon coupling strength can be covered. We show that the coupling with the phonon bath not only modifies the steady state, resulting in population inversion, but also introduces a finite steady state coherence which optimizes the energy transfer flux and efficiency. In the strong coupling limit, the steady state coherence disappears and the efficiency approaches the heat engine limit given by Scovil and Schultz-Dubois in Phys. Rew. Lett. 2, 262 (1959).
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Light harvesting components of photosynthetic organisms are complex, coupled, many-body quantum systems, in which electronic coherence has recently been shown to survive for relatively long time scales despite the decohering effects of their environments. Within this context, we analyze entanglement in multi-chromophoric light harvesting complexes, and establish methods for quantification of entanglement by presenting necessary and sufficient conditions for entanglement and by deriving a measure of global entanglement. These methods are then applied to the Fenna-Matthews-Olson (FMO) protein to extract the initial state and temperature dependencies of entanglement. We show that while FMO in natural conditions largely contains bipartite entanglement between dimerized chromophores, a small amount of long-range and multipartite entanglement exists even at physiological temperatures. This constitutes the first rigorous quantification of entanglement in a biological system. Finally, we discuss the practical utilization of entanglement in densely packed molecular aggregates such as light harvesting complexes.
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The thermodynamic properties of quantum heat engines are stochastic owing to the presence of thermal and quantum fluctuations. We here experimentally investigate the efficiency and nonequilibrium entropy production statistics of a spin-1/2 quantum Otto cycle. We first study the correlations between work and heat within a cycle by extracting their joint distribution for different driving times. We show that near perfect anticorrelation, corresponding to the tight-coupling condition, can be achieved. In this limit, the reconstructed efficiency distribution is peaked at the macroscopic efficiency and fluctuations are strongly suppressed. We further test the second law in the form of a joint fluctuation relation for work and heat. Our results characterize the statistical features of a small-scale thermal machine in the quantum domain and provide means to control them.
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