Quantum State Tuning of Energy Transfer in a Correlated Environment

Fassioli, Francesca; Nazir, Ahsan; Olaya-Castro, Alexandra

doi:10.1021/jz100717d

Cited by 108 publications

(139 citation statements)

References 30 publications

(115 reference statements)

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“…Recent studies include spatial correlations into the exciton dynamics. [38][39][40] The second-order TCL master equation for the reduced system density matrix in the interaction picture, ͑t͒, is given by…”

Section: Master Equationmentioning

confidence: 99%

Non-Markovian quantum jumps in excitonic energy transfer

Rebentrost

Chakraborty

Aspuru‐Guzik

2009

The Journal of Chemical Physics

129

166

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We utilize the novel non-Markovian quantum jump ͑NMQJ͒ approach to stochastically simulate exciton dynamics derived from a time-convolutionless master equation. For relevant parameters and time scales, the time-dependent, oscillatory decoherence rates can have negative regions, a signature of non-Markovian behavior and of the revival of coherences. This can lead to non-Markovian population beatings for a dimer system at room temperature. We show that strong exciton-phonon coupling to low frequency modes can considerably modify transport properties. We observe increased exciton transport, which can be seen as an extension of recent environment-assisted quantum transport concepts to the non-Markovian regime. Within the NMQJ method, the FennaMatthew-Olson protein is investigated as a prototype for larger photosynthetic complexes.

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Section: Master Equationmentioning

confidence: 99%

Non-Markovian quantum jumps in excitonic energy transfer

Rebentrost

Chakraborty

Aspuru‐Guzik

2009

The Journal of Chemical Physics

129

166

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“…[16][17][18][19][20][21][22] Detailed systembath interaction models have also been developed including a cross-coupling model 23 and the common bath coupling model. 8,9,[24][25][26] All of these studies so far incorporate the effects of correlation between fluctuations in the excitation energies of different sites.…”

Section: Introductionmentioning

confidence: 99%

Influence of environment induced correlated fluctuations in electronic coupling on coherent excitation energy transfer dynamics in model photosynthetic systems

Huo

Coker

2012

The Journal of Chemical Physics

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Two-dimensional photon-echo experiments indicate that excitation energy transfer between chromophores near the reaction center of the photosynthetic purple bacterium Rhodobacter sphaeroides occurs coherently with decoherence times of hundreds of femtoseconds, comparable to the energy transfer time scale in these systems. The original explanation of this observation suggested that correlated fluctuations in chromophore excitation energies, driven by large scale protein motions could result in long lived coherent energy transfer dynamics. However, no significant site energy correlation has been found in recent molecular dynamics simulations of several model light harvesting systems. Instead, there is evidence of correlated fluctuations in site energy-electronic coupling and electronic coupling-electronic coupling. The roles of these different types of correlations in excitation energy transfer dynamics are not yet thoroughly understood, though the effects of site energy correlations have been well studied. In this paper, we introduce several general models that can realistically describe the effects of various types of correlated fluctuations in chromophore properties and systematically study the behavior of these models using general methods for treating dissipative quantum dynamics in complex multi-chromophore systems. The effects of correlation between site energy and inter-site electronic couplings are explored in a two state model of excitation energy transfer between the accessory bacteriochlorophyll and bacteriopheophytin in a reaction center system and we find that these types of correlated fluctuations can enhance or suppress coherence and transfer rate simultaneously. In contrast, models for correlated fluctuations in chromophore excitation energies show enhanced coherent dynamics but necessarily show decrease in excitation energy transfer rate accompanying such coherence enhancement. Finally, for a three state model of the Fenna-Matthews-Olsen light harvesting complex, we explore the influence of including correlations in inter-chromophore couplings between different chromophore dimers that share a common chromophore. We find that the relative sign of the different correlations can have profound influence on decoherence time and energy transfer rate and can provide sensitive control of relaxation in these complex quantum dynamical open systems.

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“…Quantifying the extent to which quantum coherence enhances the performance of antennae or communication systems is a timely [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19], yet often controversial, subject. Typically, a classical system is compared to the analogous, quantised model [12,13,[20][21][22], although such a correspondence is not straightforward when open, dissipative systems are considered, as it should be in most cases of interest.…”

mentioning

confidence: 99%

“…Energy excitation transfer. We can now apply our model to the study of energy excitation transfer through the lattice [2][3][4][5][6][7][8][9][10][11][13][14][15][16] by comparing, at given local transition probabilities p and q, the performance of a classical process with that of quantum dynamics where coherent phases are allowed to develop and interfere along the chain. Note that the equality of the local transition probabilities ensures that all the difference between the classical and quantum cases is down to quantum coherence, in a very specific sense.…”

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confidence: 99%

Noisy Quantum Cellular Automata for Quantum versus Classical Excitation Transfer

Avalle

Serafini

2014

Phys. Rev. Lett.

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*We introduce a class of noisy quantum cellular automata on a qubit lattice that includes all classical Markov chains, as well as maps where quantum coherence between sites is allowed to build up over time. We apply such a construction to the problem of excitation transfer through 1-d lattices, and compare the performance of classical and quantum dynamics with equal local transition probabilities. Our discrete approach has the merits of stripping down the complications of the open system dynamics, of clearly isolating coherent effects, of allowing for an exact treatment of conditional dynamics, all while capturing a rich variety of dynamical behaviours. PACS numbers: 03.65.Yz, 03.65.Aa, Quantifying the extent to which quantum coherence enhances the performance of antennae or communication systems is a timely [1][2][3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19], yet often controversial, subject. Typically, a classical system is compared to the analogous, quantised model [12,13,[20][21][22], although such a correspondence is not straightforward when open, dissipative systems are considered, as it should be in most cases of interest.In this manuscript, we introduce a strictly local model of energy transfer via a noisy quantum cellular automaton construction [23,24] on a qubit lattice. Tuning one real parameter of such a model will allow us to range from a classical Markov chain, where quantum coherence is systematically suppressed at each time-step of the automaton, to dynamics where quantum coherence is allowed to build up over time, while keeping, by construction, the local transition probabilities constant. Thus, a "fair" comparison between classical and quantum energy transfer may be carried out, where the effect of quantum interference is singled out with no ambiguity. Our model, restricted to the first excitation subspace, can be studied exactly for very large systems, also including conditional dynamics due to measurements (which will model the absorption of the excitation at the end of the energy transfer process).The plan of the paper is as follows. We shall first consider the problem of constructing a class of one-qubit completely positive (CP) maps that, in a certain limit, reproduce all classical Markov transition matrices on dichotomic probability distributions. We will then apply our construction to the first excitation subspace of a partitioned quantum cellular automaton structure (where one-qubit maps will be applied to the two-dimensional space spanned by excitations at neighbouring sites), obtaining a global dynamics on a lattice which is capable of describing excitation transfer. We will then present a study of the performance of classical versus quantum maps, showing by how much and under what conditions does quantum coherence improve the probability of excitation transfer through the lattice. Finally, we shall draw some conclusions and discuss outlook of this work. Let us remind the reader that the matrix (and map) T p,q is referred to as doubly stochastic if p = q. Any classical...

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Quantum State Tuning of Energy Transfer in a Correlated Environment

Cited by 108 publications

References 30 publications

Non-Markovian quantum jumps in excitonic energy transfer

Non-Markovian quantum jumps in excitonic energy transfer

Influence of environment induced correlated fluctuations in electronic coupling on coherent excitation energy transfer dynamics in model photosynthetic systems

Noisy Quantum Cellular Automata for Quantum versus Classical Excitation Transfer

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