A coherent modified Redfield theory for excitation energy transfer in molecular aggregates

Hwang-Fu, Yu-Hsien; Chen, Wei; Cheng, Yuan‐Chung

doi:10.1016/j.chemphys.2014.11.026

Cited by 65 publications

(57 citation statements)

References 51 publications

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“…To describe the EET dynamics induced by the system-bath couplings, we could obtain the master equation for the CMRT as4142…”

Section: Resultsmentioning

confidence: 99%

“…The CMRT describes the quantum dynamics of EET in photosynthetic complexes over a broad parameter regime4142 and it is generalized to simulate the energy transfer in the presence of laser fields40. Furthermore, the master equation of CMRT recast in Lindblad form can be efficiency solved by the NMQJ method4445.…”

Section: Discussionmentioning

confidence: 99%

“…On the other hand, in ref. 41, the population dynamics for FMO are compared by the CMRT and HEOM. Clearly, the coherent dynamics simulated by the HEOM can be well reproduced by the CMRT.…”

Section: Discussionmentioning

confidence: 99%

“…In order to simulate the single-molecule experiment in natural photosynthetic complexes, we explore a theoretical approach40 by combining a coherent modified Redfield theory (CMRT)4142 and a non-Markovian quantum jump (NMQJ) method434445. As a generalization of the modified Redfield theory4647, the CMRT can describe a quantum system’s density matrix completely40 and has been successfully applied to simulate coherent EET dynamics in photosynthetic light harvesting414248. In 2008, Piilo and coworkers developed an efficient NMQJ method to simulate non-Markovian dynamics of an open quantum system4445.…”

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confidence: 99%

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Proposal for probing energy transfer pathway by single-molecule pump-dump experiment

Tao

Deng

et al. 2016

Sci Rep

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The structure of Fenna-Matthews-Olson (FMO) light-harvesting complex had long been recognized as containing seven bacteriochlorophyll (BChl) molecules. Recently, an additional BChl molecule was discovered in the crystal structure of the FMO complex, which may serve as a link between baseplate and the remaining seven molecules. Here, we investigate excitation energy transfer (EET) process by simulating single-molecule pump-dump experiment in the eight-molecules complex. We adopt the coherent modified Redfield theory and non-Markovian quantum jump method to simulate EET dynamics. This scheme provides a practical approach of detecting the realistic EET pathway in BChl complexes with currently available experimental technology. And it may assist optimizing design of artificial light-harvesting devices.

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“…To describe the EET dynamics induced by the system-bath couplings, we could obtain the master equation for the CMRT as4142…”

Section: Resultsmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

“…On the other hand, in ref. 41, the population dynamics for FMO are compared by the CMRT and HEOM. Clearly, the coherent dynamics simulated by the HEOM can be well reproduced by the CMRT.…”

Section: Discussionmentioning

confidence: 99%

mentioning

confidence: 99%

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Proposal for probing energy transfer pathway by single-molecule pump-dump experiment

Tao

Deng

et al. 2016

Sci Rep

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“…These effects were initially studied within a generalized Haken-Strobl-Reineker (HSR) model [15,16], where external environmental fluctuations are described in terms of classical Gaussian Markov processes (white noise). Further studies by Huo and Coker [17] performed with refined numerical techniques [18] along with more recent ones by other groups [19,20,21] using different modified quantum master equation (QME) approches showed that the same phenomenology persists also with explicit non-Markovian harmonic models of heat bath.…”

Section: Introductionmentioning

confidence: 93%

Exciton transport in the PE545 complex: insight from atomistic QM/MM-based quantum master equations and elastic network models

et al. 2017

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In this paper, we work out a parameterization of environmental noise within the Haken-Strobl-Reinenker (HSR) model for the PE545 light-harvesting complex, based on atomic-level quantum mechanics/molecular mechanics (QM/MM) simulations. We use this approach to investigate the role of various auto- and cross-correlations in the HSR noise tensor, confirming that site-energy autocorrelations (pure dephasing) terms dominate the noise-induced exciton mobility enhancement, followed by site energy-coupling cross-correlations for specific triplets of pigments. Interestingly, several cross-correlations of the latter kind, together with coupling-coupling cross-correlations, display clear low-frequency signatures in their spectral densities in the 30-70 [Formula: see text] region. These slow components lie at the limits of validity of the HSR approach, which requires that environmental fluctuations be faster than typical exciton transfer time scales. We show that a simple coarse-grained elastic-network-model (ENM) analysis of the PE545 protein naturally spotlights collective normal modes in this frequency range that represent specific concerted motions of the subnetwork of cysteines covalenty linked to the pigments. This analysis strongly suggests that protein scaffolds in light-harvesting complexes are able to express specific collective, low-frequency normal modes providing a fold-rooted blueprint of exciton transport pathways. We speculate that ENM-based mixed quantum classical methods, such as Ehrenfest dynamics, might be promising tools to disentangle the fundamental designing principles of these dynamical processes in natural and artificial light-harvesting structures.

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On the Generalization of Marcus Theory for Two‐State Photophysical Processes

Hsu,

Yang

2024

Exploring Chemical Concepts Through Theory and Computation

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A coherent modified Redfield theory for excitation energy transfer in molecular aggregates

Cited by 65 publications

References 51 publications

Proposal for probing energy transfer pathway by single-molecule pump-dump experiment

Proposal for probing energy transfer pathway by single-molecule pump-dump experiment

Exciton transport in the PE545 complex: insight from atomistic QM/MM-based quantum master equations and elastic network models

On the Generalization of Marcus Theory for Two‐State Photophysical Processes

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