An efficient method to calculate excitation energy transfer in light-harvesting systems: application to the Fenna–Matthews–Olson complex

Ritschel, Gerhard; Roden, Jan; Strunz, Walter T.; Eisfeld, Alexander

doi:10.1088/1367-2630/13/11/113034

Cited by 85 publications

(126 citation statements)

References 66 publications

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“…[19][20][21][22]). In previous works we have replaced that functional derivative by an operator ansatz and dealt with it in the so called ZOFE approximation [11,[23][24][25] that allows for a very efficient numerical solution and agrees remarkably well with established results for a large number of problems. However, in certain cases this method is known to fail (see e.g.…”

supporting

confidence: 57%

“…[7][8][9][10]. NMQSD has been applied to various physical problems including the description of energy transfer in photosynthesis [11,12]. On a more fundamental side, NMQSD has been studied in the context of continuous measurement theory [13,14] and spontaneous wavefunction localization [15].…”

mentioning

confidence: 99%

“…However, in general, approximation schemes are necessary (e.g. the ZOFE approximation [11,24]). Here we will proceed differently, without any approximation.…”

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confidence: 99%

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Hierarchy of Stochastic Pure States for Open Quantum System Dynamics

2014

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We derive a hierarchy of stochastic evolution equations for pure states (quantum trajectories) to efficiently solve open quantum system dynamics with non-Markovian structured environments. From this hierarchy of pure states (HOPS) the exact reduced density operator is obtained as an ensemble average. We demonstrate the power of HOPS by applying it to the Spin-Boson model, the calculation of absorption spectra of molecular aggregates and energy transfer in a photosynthetic pigment-protein complex.The treatment of the dynamics of realistic open quantum systems still poses both conceptual and computational challenges. These arise from non-Markovian behavior due to a structured environment or strong systemenvironment interaction [1,2]. Severe assumptions, like weak-coupling or Markov approximation, are often made for practical reasons. However, they fail for many systems of interest. In these situations one relies on computationally demanding numerical methods. Among these are path integral approaches [3,4] or hierarchical equations of motion [5,6] for the system's reduced density matrix.In this Letter we follow a different strategy and derive a hierarchy of stochastic differential equations for pure states in the system Hilbert space (quantum trajectories). From this hierarchy of pure states (HOPS) the exact reduced density operator is obtained as an ensemble average. Our approach is based upon non-Markovian Quantum State diffusion (NMQSD), derived in its general form in Refs. [7][8][9][10]. NMQSD has been applied to various physical problems including the description of energy transfer in photosynthesis [11,12]. On a more fundamental side, NMQSD has been studied in the context of continuous measurement theory [13,14] and spontaneous wavefunction localization [15]. Other stochastic approaches, with various levels of applicability have been suggested [16][17][18].Although the NMQSD approach is formally exact, it seemed numerically difficult to handle, because of the appearance of a functional derivative with respect to a stochastic process. Only a few exactly solvable models are known (see e.g. [19][20][21][22]). In previous works we have replaced that functional derivative by an operator ansatz and dealt with it in the so called ZOFE approximation [11,[23][24][25] that allows for a very efficient numerical solution and agrees remarkably well with established results for a large number of problems. However, in certain cases this method is known to fail (see e.g. [11,25]). In Ref.[26] a hierarchical approach is applied to the operator ansatz of the functional derivative. Our new HOPS presented here is not based on the previously assumed ansatz, it is numerically exact, converges rapidly and offers a systematic way to check for convergence by increasing the number of equations taken into account. In addition, it offers the advantages of stochastic Schrödinger equations, e.g. one deals with pure states (and not large density matrices) and the calculation of independent realizations can be parallelized trivially.In the ...

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Hierarchy of Stochastic Pure States for Open Quantum System Dynamics

2014

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“…In particular, the importance of structured environments in the dynamics and coherence of open quantum systems is now beginning to be recognized. For example, a series of recent theoretical [5][6][7][8][9][10][11][12] and experimental [13][14][15][16] studies has provided strong evidence that strongly coupled discrete molecular vibrations play a significant role in the speed, efficiency, and quantum coherence of energy transfer in photosynthetic and other molecular systems. In a different context, the high degree of control and precision possible in artificial nanosystems has enabled experimental measurement and engineering of noise spectral densities in condensed matter systems.…”

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confidence: 99%

Coherent exciton dynamics in a dissipative environment maintained by an off-resonant vibrational mode

2016

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The interplay between an open quantum system and its environment can lead to both coherent and incoherent behavior. We explore the extent to which strong coupling to a single bosonic mode can alter the coherence properties of a two-level system in a structured environment. This mode is treated exactly, with the rest of the environment comprising a Markovian bath of bosonic modes. The strength of the coupling between the two-level system and the single mode is varied for a variety of forms for the bath spectral density in order to assess whether the coherent dynamics of the two-level system are modified. We find a clear renormalization of the site population oscillation frequency that causes an altered interaction with the bath. This leads to enhanced or reduced coherent behavior of the two-level system, depending on the form of the spectral density function. We present an intuitive interpretation, based on an analytical model, to explain the behavior.

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“…[1][2][3][4][5][6][7][8] In particular, resonant (or near resonant) interactions between environmental degrees of freedom and those inherent to the system are thought to play an important role in numerous physical processes. [9][10][11][12][13][14][15][16][17][18][19][20] However, a comprehensive picture of such dynamics is only beginning to emerge due to the complexity of the systems in question. Here, by focusing on a proposed model for olfaction as a vibrationally-activated molecular switch, we explore the detailed effects of the environment on the dynamics of electron transfer (ET) in an open quantum system, aiming to gain physical insight into vibrationally-assisted transport processes more generally.…”

Section: Introductionmentioning

confidence: 99%

Dissipation enhanced vibrational sensing in an olfactory molecular switch

Chęcińska

Pollock

Heaney

et al. 2015

The Journal of Chemical Physics

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Motivated by a proposed olfactory mechanism based on a vibrationally-activated molecular switch, we study electron transport within a donor-acceptor pair that is coupled to a vibrational mode and embedded in a surrounding environment. We derive a polaron master equation with which we study the dynamics of both the electronic and vibrational degrees of freedom beyond previously employed semiclassical (MarcusJortner) rate analyses. We show: (i) that in the absence of explicit dissipation of the vibrational mode, the semiclassical approach is generally unable to capture the dynamics predicted by our master equation due to both its assumption of one-way (exponential) electron transfer from donor to acceptor and its neglect of the spectral details of the environment; (ii) that by additionally allowing strong dissipation to act on the odorant vibrational mode we can recover exponential electron transfer, though typically at a rate that differs from that given by the Marcus-Jortner expression; (iii) that the ability of the molecular switch to discriminate between the presence and absence of the odorant, and its sensitivity to the odorant vibrational frequency, are enhanced significantly in this strong dissipation regime, when compared to the case without mode dissipation; and (iv) that details of the environment absent from previous Marcus-Jortner analyses can also dramatically alter the sensitivity of the molecular switch, in particular allowing its frequency resolution to be improved. Our results thus demonstrate the constructive role dissipation can play in facilitating sensitive and selective operation in molecular switch devices, as well as the inadequacy of semiclassical rate equations in analysing such behaviour over a wide range of parameters.

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An efficient method to calculate excitation energy transfer in light-harvesting systems: application to the Fenna–Matthews–Olson complex

Cited by 85 publications

References 66 publications

Hierarchy of Stochastic Pure States for Open Quantum System Dynamics

Hierarchy of Stochastic Pure States for Open Quantum System Dynamics

Coherent exciton dynamics in a dissipative environment maintained by an off-resonant vibrational mode

Dissipation enhanced vibrational sensing in an olfactory molecular switch

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