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Register a new userA simple model for exploring the role of quantum coherence and the environment in excitonic energy transfer
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Sreenath Kizhakkumpurath Manikandan
Publication date
2014
fields
Physics
and research's language is
English
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We investigate the role of quantum coherence in modulating the energy transfer rate between two independent energy donors and a single acceptor participating in an excitonic energy transfer process. The energy transfer rate depends explicitly on the nature of the initial coherent superposition state of the two donors and we connect it to the observed absorption profile of the acceptor and the stimulated emission profile of the energy donors. We consider simple models with mesoscopic environments interacting with the donors and the acceptor and compare the expression we obtained for the energy transfer rate with the results of numerical integration.
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Energy transfer within photosynthetic systems can display quantum effects such as delocalized excitonic transport. Recently, direct evidence of long-lived coherence has been experimentally demonstrated for the dynamics of the Fenna-Matthews-Olson (FMO) protein complex [Engel et al., Nature 446, 782 (2007)]. However, the relevance of quantum dynamical processes to the exciton transfer efficiency is to a large extent unknown. Here, we develop a theoretical framework for studying the role of quantum interference effects in energy transfer dynamics of molecular arrays interacting with a thermal bath within the Lindblad formalism. To this end, we generalize continuous-time quantum walks to non-unitary and temperature-dependent dynamics in Liouville space derived from a microscopic Hamiltonian. Different physical effects of coherence and decoherence processes are explored via a universal measure for the energy transfer efficiency and its susceptibility. In particular, we demonstrate that for the FMO complex an effective interplay between free Hamiltonian and thermal fluctuations in the environment leads to a substantial increase in energy transfer efficiency from about 70% to 99%.
We demonstrate that the coupling of excitonic and vibrational motion in biological complexes can provide mechanisms to explain the long-lived oscillations that have been obtained in non linear spectroscopic signals of different photosynthetic pigment protein complexes and we discuss the contributions of excitonic versus purely vibrational components to these oscillatory features. Considering a dimer model coupled to a structured spectral density we exemplify the fundamental aspects of the electron-phonon dynamics, and by analyzing separately the different contributions to the non linear signal, we show that for realistic parameter regimes purely electronic coherence is of the same order as purely vibrational coherence in the electronic ground state. Moreover, we demonstrate how the latter relies upon the excitonic interaction to manifest. These results link recently proposed microscopic, non-equilibrium mechanisms to support long lived coherence at ambient temperatures with actual experimental observations of oscillatory behaviour using 2D photon echo techniques to corroborate the fundamental importance of the interplay of electronic and vibrational degrees of freedom in the dynamics of light harvesting aggregates.
We discuss the role of quantum coherence in the energy fluctuations of open quantum systems. To this aim, we introduce an operational protocol, to which we refer to as the end-point-measurement scheme, allowing to define the statistics of energy changes as a function of energy measurements performed only after its evolution. At the price of an additional uncertainty on the value of the initial energies, this approach prevents the loss of initial quantum coherences and enables the estimation of their effects on energy fluctuations. We illustrate our findings using a three-level quantum system in interaction with thermal reservoirs.
We discuss the role of quantum coherence in the energy fluctuations of open quantum systems. To this aim, we introduce a protocol, to which we refer to as the end-point-measurement scheme, allowing to define the statistics of energy changes as a function of energy measurements performed only after the evolution of the initial state. At the price of an additional uncertainty on the initial energies, this approach prevents the loss of initial quantum coherences and enables the estimation of their effects on energy fluctuations. We demonstrate our findings by running an experiment on the IBM Quantum Experience superconducting qubit platform.
The role of quantum coherence and the environment in the dynamics of excitation energy transfer is not fully understood. In this work, we introduce the concept of dynamical contributions of various physical processes to the energy transfer efficiency. We develop two complementary approaches, based on a Greens function method and energy transfer susceptibilities, and quantify the importance of the Hamiltonian evolution, phonon-induced decoherence, and spatial relaxation pathways. We investigate the Fenna-Matthews-Olson protein complex, where we find a contribution of coherent dynamics of about 10% and of relaxation of 80%.
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