Theoretical Study on the Effect of Environment on Excitation Energy Transfer in Photosynthetic Light-Harvesting Systems

Cui, XueYan; Yan, YiJing; Wei, Jianhua

doi:10.1021/acs.jpcb.0c00266

Cited by 15 publications

(24 citation statements)

References 49 publications

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“…To get rid of this reverse excitation transfer, site 6 needs to quickly transfer the excitation energy to other sites. According to our previous research, 38 when site 6 is initially excited, the strongly coherent oscillations first occur between site 6 and site 5, and then the excitation energy is gradually transferred to site 4, site 7, and finally to site 3. By the analysis of the research results, we find that BChl 6 is strongly coupled to BChl 5, BChl 4, and BChla 7.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Aghtar et al suggested that environmental fluctuation has an important effect on spectral density. Besides, extensive investigations − have been carried out to study the robustness of the FMO complex with fluctuations in the surrounding protein environment, showing that the thermal fluctuation can enhance the EET by the so-called environment-assisted quantum transport.…”

Section: Introductionmentioning

confidence: 99%

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Role of Pigment–Protein Coupling in the Energy Transport Dynamics in the Fenna–Matthews–Olson Complex

2021

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The role of pigment–protein coupling in the dynamics of photosynthetic energy transport in chromophoric complexes has not been fully understood. The excitation energy transfer in the photosynthetic system is tremendously efficient. In particular, we investigate the excitation energy transport in the Fenna–Matthews–Olson (FMO) complex. The exciton dynamics and excitation energy transfer (EET) depend on the interaction between the excited chromophores and their environment. Most theoretical models believe that all bacteriochlorophyll-a (BChla) sites are surrounded by the same local protein environment, which is contradicted by the structural analysis of the FMO complex. Based on different values of pigment–protein coupling for different sites, measured in the adiabatic limit, we have theoretically investigated the effect of the heterogeneous local protein environment on the EET process. By the realistic and site-dependent model of the system–bath couplings, the results show that this interaction may have a critical value for the coherent energy-transfer process. Furthermore, we verify that the two transport pathways are coherent and stable to the important parameter reorganization energy of environmental interactions. The quantum dynamical simulations show that the correlation fluctuation keeps the oscillation of the coherent excitation on a long timescale. In addition, due to the inhomogeneous pigment–protein coupling, different BChl sites have asymmetric excitation oscillation timescales.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Role of Pigment–Protein Coupling in the Energy Transport Dynamics in the Fenna–Matthews–Olson Complex

2021

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“…Experimentally, the eighth BChl pigment has also been newly resolved in the FMO protein that lies perpendicular to the plane of the other seven BChls [17,18]. Notably, FMO complex is a homotrimer of three ≈ 40 kDa monomer that possesses C3 symmetry whereby three copies of each subunit of seven BChl a chromophores bind together to the eighth BChl a pigment [16,19,20]. Due to close packing of BChl a pigments in each monomer subunit, the excited electronic states of FMO complexes are delocalized over multiple pigments.…”

Section: Introductionmentioning

confidence: 99%

“…Due to close packing of BChl a pigments in each monomer subunit, the excited electronic states of FMO complexes are delocalized over multiple pigments. The previous research in this field is mainly focused on developing and testing new computational and experimental methods for a better understanding of the delocalization of excited states over multiple pigments and the unfolding of the relationship between atomic structure and absorbance along with the fluorescence spectra [19,20]. Owing to the rotational symmetric of the monomer subunit of FMO trimer around the symmetry axis, there are two types of FMO complex structures widely analyzed in the literature.…”

Section: Introductionmentioning

confidence: 99%

Analysis of Photosynthetic Systems and Their Applications with Mathematical and Computational Models

2020

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In biological and life science applications, photosynthesis is an important process that involves the absorption and transformation of sunlight into chemical energy. During the photosynthesis process, the light photons are captured by the green chlorophyll pigments in their photosynthetic antennae and further funneled to the reaction center. One of the most important light harvesting complexes that are highly important in the study of photosynthesis is the membrane-attached Fenna–Matthews–Olson (FMO) complex found in the green sulfur bacteria. In this review, we discuss the mathematical formulations and computational modeling of some of the light harvesting complexes including FMO. The most recent research developments in the photosynthetic light harvesting complexes are thoroughly discussed. The theoretical background related to the spectral density, quantum coherence and density functional theory has been elaborated. Furthermore, details about the transfer and excitation of energy in different sites of the FMO complex along with other vital photosynthetic light harvesting complexes have also been provided. Finally, we conclude this review by providing the current and potential applications in environmental science, energy, health and medicine, where such mathematical and computational studies of the photosynthesis and the light harvesting complexes can be readily integrated.

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“…The dissipative excited state dynamics of molecular aggregates is often treated by separating the relevant system from an environment [1,2]. The latter is usually identified with a thermal bath of low-frequency modes of the surrounding molecular matrix, such as a protein scaffold [3][4][5], but can also comprise intramolecular vibrational modes of monomers in the aggregate [6][7][8][9][10][11]. In the "Hierarchical Equations of Motion" (HEOM) method all nuclear degrees of freedom are attributed to the environment [12], and all orders of perturbation theory with respect to their interaction with the system built from purely electronic components are taken into account at least in principle [13].…”

Section: Introductionmentioning

confidence: 99%

Exciton Transfer Using Rates Extracted From the "Hierarchical Equations of Motion''

Seibt,

Kühn

2020

Preprint

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Frenkel exciton population dynamics of an excitonic dimer is studied by comparing results from a quantum master equation (QME) involving rates from second-order perturbative treatment with respect to the excitonic coupling with non-perturbative results from "Hierarchical Equations of Motion" (HEOM). By formulating generic Liouville-space expressions for the rates, we can choose to evaluate them either via HEOM propagations or by applying cumulant expansion. The coupling of electronic transitions to bath modes is modeled either as overdamped oscillators for description of thermal bath components or as underdamped oscillators to account for intramolecular vibrations. Cases of initial nonequilibrium and equilibrium vibrations are discussed. In case of HEOM initial equilibration enters via a polaron transformation. Pointing out the differences between the nonequilibrium and equilibrium approach in the context of the projection operator formalism, we identify a further description, where the transfer dynamics is driven only by fluctuations without involvement of dissipation. Despite this approximation, also this approach can yield meaningful results in certain parameter regimes. While for the chosen model HEOM has no technical advantage for evaluation of the rate expressions compared to cumulant expansion, there are situations where only evaluation with HEOM is applicable. For instance, a separation of reference and interaction Hamiltonian via a polaron transformation to account for the interplay between Coulomb coupling and vibrational oscillations of the bath at the level of a second-order treatment can be adjusted for a treatment with HEOM.

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Theoretical Study on the Effect of Environment on Excitation Energy Transfer in Photosynthetic Light-Harvesting Systems

Cited by 15 publications

References 49 publications

Role of Pigment–Protein Coupling in the Energy Transport Dynamics in the Fenna–Matthews–Olson Complex

Role of Pigment–Protein Coupling in the Energy Transport Dynamics in the Fenna–Matthews–Olson Complex

Analysis of Photosynthetic Systems and Their Applications with Mathematical and Computational Models

Exciton Transfer Using Rates Extracted From the "Hierarchical Equations of Motion''

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