Instantaneous Mapping of Coherently Coupled Electronic Transitions and Energy Transfers in a Photosynthetic Complex Using Angle-Resolved Coherent Optical Wave-Mixing

Mercer, Ian P.; El-Taha, Yasin C.; Kajumba, N.; Marangos, Jonathan P.; Tisch, J. W. G.; Gabrielsen, Mads; Cogdell, Richard J.; Springate, E.; Turcu, Edmund

doi:10.1103/physrevlett.102.057402

Cited by 81 publications

(88 citation statements)

References 18 publications

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“…Cross peaks with oscillating amplitudes are most often signatures of intramolecular vibrational modes (vibrational coherence) or strong electronic coupling (electronic coherence) [41,42,[49][50][51][52]. Similar coherent oscillations have been observed in photosynthetic proteins using related techniques as well [53][54][55][56]. The measured coherences have evoked questions about energy transfer in the intermediate-coupling regime in biological systems and even larger questions about the nature of photosynthetic complexes [57][58][59][60].…”

Section: Introductionmentioning

confidence: 91%

Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis

Turner

Howey²,

Sutor³

et al. 2012

J. Phys. Chem. A

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Electronic energy transfer in photosynthesis occurs over a range of time scales and under a variety of intermolecular coupling conditions. Recent work has shown that electronic coupling between chromophores can lead to coherent oscillations in two-dimensional electronic spectroscopy measurements of pigment-protein complexes measured with femtosecond laser pulses. A persistent issue in the field is to reconcile the results of measurements performed using femtosecond laser pulses with physiological illumination conditions. Noisy-light spectroscopy can begin to address this question. In this work we present the theoretical analysis of incoherent two-dimensional electronic spectroscopy, I(4) 2D ES. Simulations reveal diagonal peaks, cross peaks, and coherent oscillations similar to those observed in femtosecond two-dimensional electronic spectroscopy experiments. The results also expose fundamental differences between the femtosecond-pulse and noisy-light techniques; the differences lead to new challenges and new opportunities.

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Section: Introductionmentioning

confidence: 91%

Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis

Turner

Howey²,

Sutor³

et al. 2012

J. Phys. Chem. A

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“…A fascinating series of recent experiments demonstrating signatures of quantum coherence in the energy transfer dynamics of a variety of systems [1][2][3][4][5][6][7][8][9] has sparked renewed interest in modeling excitation energy transfer beyond standard methods. [10][11][12][13][14][15][16][17][18][19] This process, which occurs when energy absorbed at one site (the donor) is transferred to another nearby site (the acceptor) via a virtual photon, 20 is often considered to be incoherent; the result of weak donor-acceptor interactions, treated perturbatively using Fermi's golden rule.…”

Section: Introductionmentioning

confidence: 99%

Coherent and incoherent dynamics in excitonic energy transfer: Correlated fluctuations and off-resonance effects

2011

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We study the nature of the energy transfer process within a pair of coupled two-level systems (donor and acceptor) subject to interactions with the surrounding environment. Going beyond a standard weak-coupling approach, we derive a master equation within the polaron representation that allows for the investigation of both weak and strong system-bath couplings, as well as reliable interpolation between these two limits. With this theory, we are then able to explore both coherent and incoherent regimes of energy transfer within the donor-acceptor pair. We elucidate how the degree of correlation in the donor and acceptor fluctuations, the donor-acceptor energy mismatch, and the range of the environment frequency distribution impact upon the energy transfer dynamics. In the resonant case (no energy mismatch) we describe in detail how a crossover from coherent to incoherent transfer dynamics occurs with increasing temperature [A. Nazir, Phys. Rev. Lett. 103, 146404 (2009)], and we also explore how fluctuation correlations are able to protect coherence in the energy transfer process. We show that a strict crossover criterion is harder to define when off-resonance, though we find qualitatively similar population dynamics to the resonant case with increasing temperature, while the amplitude of coherent population oscillations also becomes suppressed with growing site energy mismatch.

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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.…”

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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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Instantaneous Mapping of Coherently Coupled Electronic Transitions and Energy Transfers in a Photosynthetic Complex Using Angle-Resolved Coherent Optical Wave-Mixing

Cited by 81 publications

References 18 publications

Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis

Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis

Coherent and incoherent dynamics in excitonic energy transfer: Correlated fluctuations and off-resonance effects

Noisy Quantum Cellular Automata for Quantum versus Classical Excitation Transfer

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