Symmetry-enhanced supertransfer of delocalized quantum states

Coherent hopping of excitation rely on quantum coherence over physically extended states. In this work, we consider simple models to examine the effect of symmetries of delocalized multi-excitation states on the dynamical timescales, including hopping rates, radiative decay, and environmental interactions. While the decoherence (pure dephasing) rate of an extended state over N sites is comparable to that of a non-extended state, superradiance leads to a factor of N enhancement in decay and absorption rates. In addition to superradiance, we illustrate how the multi-excitonic states exhibit `supertransfer' in the far-field regime: hopping from a symmetrized state over N sites to a symmetrized state over M sites at a rate proportional to MN. We argue that such symmetries could play an operational role in physical systems based on the competition between symmetry-enhanced interactions and localized inhomogeneities and environmental interactions that destroy symmetry. As an example, we propose that supertransfer and coherent hopping play a role in recent observations of anomolously long diffusion lengths in nano-engineered assembly of light-harvesting complexes.Comment: 6 page

Numerical Evidence for Robustness of Environment-Assisted Quantum Transport

Recent theoretical studies show that decoherence process can enhance transport efficiency in quantum systems. This effect is known as environment-assisted quantum transport (ENAQT). The role of ENAQT in optimal quantum transport is well investigated, however, it is less known how robust ENAQT is with respect to variations in the system or its environment characteristic. Toward answering this question, we simulated excitonic energy transfer in Fenna-Matthews-Olson (FMO) photosynthetic complex. We found that ENAQT is robust with respect to many relevant parameters of environmental interactions and Frenkel-exciton Hamiltonian including reorganization energy, bath frequency cutoff, temperature, and initial excitations, dissipation rate, trapping rate, disorders, and dipole moments orientations. Our study suggests that the ENAQT phenomenon can be exploited in robust design of highly efficient quantum transport systems.Comment: arXiv admin note: substantial text overlap with arXiv:1104.481

Geometrical effects on energy transfer in disordered open quantum systems

We explore various design principles for efficient excitation energy transport in complex quantum systems. We investigate energy transfer efficiency in randomly disordered geometries consisting of up to 20 chromophores to explore spatial and spectral properties of small natural/artificial Light-Harvesting Complexes (LHC). We find significant statistical correlations among highly efficient random structures with respect to ground state properties, excitonic energy gaps, multichromophoric spatial connectivity, and path strengths. These correlations can even exist beyond the optimal regime of environment-assisted quantum transport. For random configurations embedded in spatial dimensions of 30 A and 50 A, we observe that the transport efficiency saturates to its maximum value if the systems contain 7 and 14 chromophores respectively. Remarkably, these optimum values coincide with the number of chlorophylls in (Fenna-Matthews-Olson) FMO protein complex and LHC II monomers, respectively, suggesting a potential natural optimization with respect to chromophoric density.Comment: 11 pages, 10 figures. Expanded from the former appendix to arXiv:1104.481

Efficient estimation of nearly sparse many-body quantum Hamiltonians

We develop an efficient and robust approach to Hamiltonian identification for multipartite quantum systems based on the method of compressed sensing. This work demonstrates that with only O(s log(d)) experimental configurations, consisting of random local preparations and measurements, one can estimate the Hamiltonian of a d-dimensional system, provided that the Hamiltonian is nearly s-sparse in a known basis. We numerically simulate the performance of this algorithm for three- and four-body interactions in spin-coupled quantum dots and atoms in optical lattices. Furthermore, we apply the algorithm to characterize Hamiltonian fine structure and unknown system-bath interactions.Comment: 8 pages, 2 figures. Title is changed. Detailed error analysis is added. Figures are updated with additional clarifying discussion

Energy-scales convergence for optimal and robust quantum transport in photosynthetic complexes

Underlying physical principles for the high efficiency of excitation energy transfer in light-harvesting complexes are not fully understood. Notably, the degree of robustness of these systems for transporting energy is not known considering their realistic interactions with vibrational and radiative environments within the surrounding solvent and scaffold proteins. In this work, we employ an efficient technique to estimate energy transfer efficiency of such complex excitonic systems. We observe that the dynamics of the Fenna-Matthews-Olson (FMO) complex leads to optimal and robust energy transport due to a convergence of energy scales among all important internal and external parameters. In particular, we show that the FMO energy transfer efficiency is optimum and stable with respect to the relevant parameters of environmental interactions and Frenkel-exciton Hamiltonian including reorganization energy $\lambda$, bath frequency cutoff $\gamma$, temperature $T$, bath spatial correlations, initial excitations, dissipation rate, trapping rate, disorders, and dipole moments orientations. We identify the ratio of \lambda T/\gamma\*g as a single key parameter governing quantum transport efficiency, where g is the average excitonic energy gap.Comment: minor revisions, removing some figures, 19 pages, 19 figure

Efficient estimation of energy transfer efficiency in light-harvesting complexes

The fundamental physical mechanisms of energy transfer in photosynthetic complexes is not yet fully understood. In particular, the degree of efficiency or sensitivity of these systems for energy transfer is not known given their non-perturbative and non-Markovian interactions with proteins backbone and surrounding photonic and phononic environments. One major problem in studying light-harvesting complexes has been the lack of an efficient method for simulation of their dynamics in biological environments. To this end, here we revisit the second-order time-convolution (TC2) master equation and examine its reliability beyond extreme Markovian and perturbative limits. In particular, we present a derivation of TC2 without making the usual weak system-bath coupling assumption. Using this equation, we explore the long time behaviour of exciton dynamics of Fenna-Matthews-Olson (FMO) protein complex. Moreover, we introduce a constructive error analysis to estimate the accuracy of TC2 equation in calculating energy transfer efficiency, exhibiting reliable performance for environments with weak and intermediate memory and strength. Furthermore, we numerically show that energy transfer efficiency is optimal and robust for the FMO protein complex of green sulphur bacteria with respect to variations in reorganization energy and bath correlation time-scales.Comment: 16 pages, 9 figures, modified version, updated appendices and reference lis

Polynomial-time quantum algorithm for the simulation of chemical dynamics

The computational cost of exact methods for quantum simulation using classical computers grows exponentially with system size. As a consequence, these techniques can only be applied to small systems. By contrast, we demonstrate that quantum computers could exactly simulate chemical reactions in polynomial time. Our algorithm uses the split-operator approach and explicitly simulates all electron-nuclear and inter-electronic interactions in quadratic time. Surprisingly, this treatment is not only more accurate than the Born-Oppenheimer approximation, but faster and more efficient as well, for all reactions with more than about four atoms. This is the case even though the entire electronic wavefunction is propagated on a grid with appropriately short timesteps. Although the preparation and measurement of arbitrary states on a quantum computer is inefficient, here we demonstrate how to prepare states of chemical interest efficiently. We also show how to efficiently obtain chemically relevant observables, such as state-to-state transition probabilities and thermal reaction rates. Quantum computers using these techniques could outperform current classical computers with one hundred qubits.Comment: 9 pages, 3 figures. Updated version as appears in PNA

Optimal number of pigments in photosynthetic complexes

We study excitation energy transfer in a simple model of photosynthetic complex. The model, described by Lindblad equation, consists of pigments interacting via dipole-dipole interaction. Overlapping of pigments induces an on-site energy disorder, providing a mechanism for blocking the excitation transfer. Based on the average efficiency as well as robustness of random configurations of pigments, we calculate the optimal number of pigments that should be enclosed in a pigment-protein complex of a given size. The results suggest that a large fraction of pigment configurations are efficient as well as robust if the number of pigments is properly chosen. We compare optimal results of the model to the structure of pigment-protein complexes as found in nature, finding good agreement.Comment: 20 pages, 7 figures; v2.: new appendix, published versio

Environment-Assisted Quantum Transport

Transport phenomena at the nanoscale are of interest due to the presence of both quantum and classical behavior. In this work, we demonstrate that quantum transport efficiency can be enhanced by a dynamical interplay of the system Hamiltonian with pure dephasing induced by a fluctuating environment. This is in contrast to fully coherent hopping that leads to localization in disordered systems, and to highly incoherent transfer that is eventually suppressed by the quantum Zeno effect. We study these phenomena in the Fenna-Matthews-Olson protein complex as a prototype for larger photosynthetic energy transfer systems. We also show that disordered binary tree structures exhibit enhanced transport in the presence of dephasing.Comment: 7 pages, 3 figures, improved presentation, to appear in New Journal of Physic

Environment-Assisted Quantum Walks in Photosynthetic Energy Transfer

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%.Comment: 9 pages, 3 figures, improved presentation, updated references, to appear in Journal of Chemical Physic