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Register a new userQuantum effects in energy and charge transfer in an artificial photosynthetic complex
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Added by
Pulak Kumar Ghosh Dr.
Publication date
2011
fields
Physics
and research's language is
English
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We investigate the quantum dynamics of energy and charge transfer in a wheel-shaped artificial photosynthetic antenna-reaction center complex.This complex consists of six light-harvesting chromophores and an electron-acceptor fullerene. To describe quantum effects on a femtosecond time scale, we derive the set of exact non-Markovian equations for the Heisenberg operators of this photosynthetic complex in contact with a Gaussian heat bath. With these equations we can analyze the regime of strong system-bath interactions, where reorganization energies are of the order of the intersite exciton couplings. We show that the energy of the initially-excited antenna chromophores is efficiently funneled to the porphyrin-fullerene reaction center, where a charge-separated state is set up in a few picoseconds, with a quantum yield of the order of 95%. In the single-exciton regime, with one antenna chromophore being initially excited, we observe quantum beatings of energy between two resonant antenna chromophores with a decoherence time of $sim$ 100 fs. We also analyze the double-exciton regime, when two porphyrin molecules involved in the reaction center are initially excited. In this regime we obtain pronounced quantum oscillations of the charge on the fullerene molecule with a decoherence time of about 20 fs (at liquid nitrogen temperatures). These results show a way to directly detect quantum effects in artificial photosynthetic systems.
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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%.
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.
Several recent studies of energy transfer in photosynthetic light harvesting complexes have revealed a subtle interplay between coherent and decoherent dynamic contributions to the overall transfer efficiency in these open quantum systems. In this work we systematically investigate the impact of temporal and spatial correlations in environmental fluctuations on excitation transport in the Fenna-Matthews-Olson photosynthetic complex. We demonstrate that the exact nature of the correlations can have a large impact on the efficiency of light harvesting. In particular, we find that (i) spatial correlations can enhance coherences in the site basis while at the same time slowing transport, and (ii) the overall efficiency of transport is optimized at a finite temporal correlation that produces maximum overlap between the environmental power spectrum and the excitonic energy differences, which in turn results in enhanced driving of transitions between excitonic states.
We analyze a theoretical model for energy and electron transfer in an artificial photosynthetic system. The photosystem consists of a molecular triad (i.e., with a donor, a photosensitive unit, and an acceptor) coupled to four accessory light-harvesting antennas pigments. The excitation energy transfer from the antennas to the artificial reaction center (the molecular triad) is here described by the F{o}rster mechanism. We consider two different kinds of arrangements of the accessory light-harvesting pigments around the reaction center. The first arrangement allows direct excitation transfer to the reaction center from all the surrounding pigments. The second configuration transmits energy via a cascade mechanism along a chain of light-harvesting chromophores, where only one chromophore is connected to the reaction center. At first sight, it would appear that the star-shaped configuration, with all the antennas directly coupled to the photosensitive center, would be more efficient. However, we show that the artificial photosynthetic system using the cascade energy transfer absorbs photons in a broader wavelength range and converts their energy into electricity with a higher efficiency than the system based on direct couplings between all the antenna chromophores and the reaction center.
We study a model of a light-induced proton pump in artificial reaction centers. The model contains a molecular triad with four electron states (i.e., one donor state, two photosensitive group states, and one acceptor state) as well as a molecular shuttle having one electron and one proton-binding sites. The shuttle diffuses between the sides of the membrane and translocates protons energetically uphill: from the negative side to the positive side of the membrane, harnessing for this purpose the energy of the electron-charge-separation produced by light. Using methods of quantum transport theory we calculate the range of light intensity and transmembrane potentials that maximize both the light-induced proton current and the energy transduction efficiency. We also study the effect of temperature on proton pumping. The light-induced proton pump in our model gives a quantum yield of proton translocation of about 55 %. Thus, our results explain previous experiments on these artificial photosynthetic reaction centers.
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