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Journal of Physics B Atomic Molecular and Optical Physics

New approach to energy transfer and quantum correlations in a molecular dimer

M Saberi, M. Bagheri Harouni, R. Roknizadeh, Hamid Latifi

Published Sep 5, 2016• 0 citations
Publisher

Abstract

Abstract The dynamics of single-excitation energy transfer in a molecular dimer interacting with a phonon bath is studied. Although there are exact numerical solutions for this system, we propose an approach that provides exact analytical results with few electronic degrees of freedom. This approach is based on considering the phonon subsystem in the coherent state representation. Applying this approach, the long-lived coherence time is evaluated in the weak and strong coupling regimes. Moreover, by calculating the quantum entanglement and global quantum discord, the time evolution of quantum correlations is examined. The effects of two parameters, electronic coupling strength and bath temperature, on the energy transfer and quantum correlations are studied. It is shown, in agreement with previous results, that the long-lived coherence time in the weak coupling regime is longer than in the strong coupling regime. Also, the increasing bath temperature gives rise to faster delocalization of energy transfer. Furthermore, it is illustrated that the bath temperature has a significant effect on the quantum entanglement with respect to the global quantum discord.

DOI
10.1088/0953-4075/49/18/185501

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•Sep 1, 2015•1 citation
Abstract The dynamics of single-excitation energy transfer in a molecular dimer interacting with a phonon bath is studied. Although there are exact numerical solutions for this system, we propose an approach that provides exact analytical results with few electronic degrees of freedom. This approach is based on considering the phonon subsystem in the coherent state representation. Applying this approach, the long-lived coherence time is evaluated in the weak and strong coupling regimes. Moreover, by calculating the quantum entanglement and global quantum discord, the time evolution of quantum correlations is examined. The effects of two parameters, electronic coupling strength and bath temperature, on the energy transfer and quantum correlations are studied. It is shown, in agreement with previous results, that the long-lived coherence time in the weak coupling regime is longer than in the strong coupling regime. Also, the increasing bath temperature gives rise to faster delocalization of energy transfer. Furthermore, it is illustrated that the bath temperature has a significant effect on the quantum entanglement with respect to the global quantum discord.
In this paper, a new analytical approach for the dynamics of excitation energy transfer and quantum entanglement in a photosynthetic dimer system is presented. In this approach, the protein environment is investigated as a phonon bath and the coherent representation is investigated to display of their states. The exact analytical expressions for the population of two pigments and their quantum entanglement is obtained. It is shown that numerical results have a good matching with the experimental results for both limits of weak and strong electronic coupling at cryogenic and physiological temperatures.
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We study coherent energy transfer of a single excitation and quantum entanglement in a dimer, which consists of a donor and an acceptor modeled by two two-level systems. Between the donor and the acceptor, there exists a dipole-dipole interaction, which provides the physical mechanism for coherent energy transfer and entanglement generation. The donor and the acceptor couple to two independent heat baths with diagonal couplings that do not dissipate the energy of the noncoupling dimer. Special attention is paid to the effect on single-excitation energy transfer and entanglement generation of the energy detuning between the donor and the acceptor and the temperatures of the two heat baths. It is found that, the probability for single-excitation energy transfer largely depends on the energy detuning in the low temperature limit. Concretely, the positive and negative energy detunings can increase and decrease the probability at steady state, respectively. In the high temperature limit, however, the effect of the energy detuning on the probability is negligibly small. We also find that the probability is negligibly dependent on the bath temperature difference of the two heat baths. In addition, it is found that quantum entanglement can be generated in the process of coherent energy transfer. As the bath temperature increases, the generated steady-state entanglement decreases. For a given bath temperature, the steady-state entanglement decreases with the increase of the absolute value of the energy detuning.
Dynamics of the quantum entanglement and quantum discord of two qubits in two independent baths and a common bath with the Lorentzian spectrum are studied exactly in the numerical sense within the hierarchy approach. The effects of the counter-rotating-wave terms from the system–bath coherence on these quantum correlations are systematically discussed and comparisons with previous ones under the rotating-wave approximation are also performed. For two independent baths, beyond the weak system–bath coupling, the counter-rotating-wave terms essentially change evolutions of both the entanglement and quantum discord. With increase of the coupling, revival of the entanglement after a period of complete disentanglement is suppressed dramatically and finally disappears, and the quantum discord becomes smaller monotonically. For the common bath, the entanglement is also suppressed by the counter-rotating-wave terms, but the quantum discord shows quite different behaviors if initiated from spin-correlated states. In the non-Markovian regime, the quantum discord is almost not influenced by the counter-rotating-wave terms and is generally finite in the long-time evolution at arbitrary coupling while in the Markovian regime, it is significantly enhanced with the strong coupling.
The quantum entanglement, discord, and coherence dynamics of two spins in the model of a spin coupled to a spin bath through an intermediate spin are studied. The effects of the important physical parameters including the coupling strength of two spins, the interaction strength between the intermediate spin and the spin bath, the number of bath spins and the temperature of the system on quantum coherence and correlation dynamics are discussed in different cases. The frozen quantum discord can be observed whereas coherence does not when the initial state is the Bell-diagonal state. At finite temperature, we find that coherence is more robust than quantum discord, which is better than entanglement, in terms of resisting the influence of environment. Therefore, quantum coherence is more tenacious than quantum correlation as an important resource.
Strong coupling between a quantum system and its many-body environment is becoming an increasingly important topic for many branches of physics. Numerous systems of experimental and technological relevance demonstrate strong system-environment coupling, leading to complex dynamical behaviour. This thesis is concerned with two particular examples of such systems, namely quantum dots (QDs) and excitonic energy transfer (EET) in molecular systems. Traditional quantum optics treatments are often insufficient to describe the transient, steady state, and optical properties of QDs due to system-environment correlations. In contrast, we present a modified theory of quantum optics capable of capturing the influence of a thermal environment on the behaviour of QDs. Using this framework we demonstrate a striking departure of the emission spectra and photon measurement statistics of a classically driven QD when compared to an analogous atomic system. Furthermore, in contradiction to accepted notions of decoherence and dissipation, we show that the interaction between a QD and its thermal environment induces non-classical light-matter correlations in an otherwise semi-classical regime of cavity quantum electrodynamics. Away from QDs, we develop the reaction coordinate (RC) formalism to describe the dynamics of a system coupled to a low frequency environment — a regime important to EET systems. We do so by identifying and incorporating important environmental degrees of freedom into an enlarged system Hamiltonian. Uniquely, this approach gives insight directly into the dynamical evolution of the environment and correlations accumulated between the system and environment. Furthermore, it is demonstrated that these corre- lations persist into the steady state, generating non-canonical equilibrium states of the system and environment. We then apply the RC model to describe EET in a molecular dimer, highlighting the effect that under- and over-damped environments have on the excitation dynamics. In doing so, we show interactions between the dimer and a structured environment can significantly enhance the energy transfer rate.