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Register a new userUnraveling excitation energy transfer assisted by collective behaviors of vibrations
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We investigate how collective behaviors of vibrations such as cooperativity and interference can enhance energy transfer in a nontrivial way, focusing on an example of a donor-bridge-acceptor trimeric chromophore system coupled to two vibrational degrees of freedom. Employing parameters selected to provide an overall uphill energy transfer from donor to acceptor, we use numerical calculations of dynamics in a coupled exciton-vibration basis, together with perturbation-based analytics and calculation of vibronic spectra, we identify clear spectral features of single- and multi-phonon vibrationally-assisted energy transfer (VAET) dynamics, where the latter include up to six-phonon contributions. We identify signatures of vibrational cooperation and interference that provide enhancement of energy transfer relative to that obtained from VAET with a single vibrational mode. We observe a phononic analogue of two-photon absorption, as well as a novel heteroexcitation mechanism in which a single phonon gives rise to simultaneous excitation of both the trimeric system and the vibrational degrees of freedom. The impact of vibrations and of the one- and two-phonon VAET processes on the energy transfer are seen to be quite different in the weak and strong site-vibration coupling regimes. In the weak coupling regime, two-phonon processes dominate, whereas in the strong coupling regime up to six-phonon VAET processes can be induced. The VAET features are seen to be enhanced with increasing temperature and site-vibration coupling strength, and are reduced in the presence of dissipation. We analyze the dependence of these phenomena on the explicit form of the chromophore-vibration couplings, with comparison of VAET spectra for local and non-local couplings.
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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%.
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.
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.
Motivated by recent experiments on photon statistics from individual dye pairs planted on biomolecules and coupled by fluorescence resonance energy transfer (FRET), we show here that the FRET dynamics can be modelled by Gaussian random processes with colored noise. Using Monte-Carlo numerical simulations, the photon intensity correlations from the FRET pairs are calculated, and are turned out to be very close to those observed in experiment. The proposed stochastic description of FRET is consistent with existing theories for microscopic dynamics of the biomolecule that carries the FRET coupled dye pairs.
Enhancement of the sensitivities of optical magnetometers, atomic clocks and atom interferometers and other quantum metrology devices requires introducing new physical processes to improve on their present achievements. Many body collective correlations among the atoms, spins or, in general, quantum systems may prove to be a suitable method. As these correlations introduce interference terms in the intensity of the scattering amplitudes, they may enhance the signal as $N(N-1)$ for N correlated quantum systems. These correlations enhance the signal to noise ratio by a factor of $N^2$ and contribute to better sensitivity in quantum metrology. Moreover atomic correlation may provide quantum noise limit, Heisenberg limit. In the present communication excitation exchange induced by photons in a cavity between two atoms is calculated and clearly exhibits correlation and collective effects. A novel operator is introduced that expresses photon-induced excitation exchange that takes in account energy conservation, $V_{ij}=hat{a}^dagsigma_isigma_j^daghat{a}$, $sigma_i=left|grightrangle_{i}leftlangle eright|_{i}$ is lowering operator of $i$-th atom, and $hat{a}^dag,hat{a}$ are photon creation and annihilation operators. Here $i$ and $j$ stand for two atoms. This operator describes real or virtual photon assisted dipole-dipole interaction. Moreover, it conserves the total number of excitations in the joint em field and the quantum system. Experimental challenges are suggested.
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