Effects of Herzberg–Teller vibronic coupling on coherent excitation energy transfer

Zhang, Hou-Dao; Qiao, Qin; Xu, Rui-Xue; Yan, YiJing

doi:10.1063/1.4968031

Cited by 43 publications

(43 citation statements)

References 64 publications

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“…At the same time, long-lived oscillatory features were observed, initially in the FMO complex 13 and later in LHCII 9 . Since then, the origin of these oscillations has been extensively debated [14][15][16][17][18][19][20][21][22][23][24][25][26] . Beyond this debate lies an even more challenging question-how does the observation of these beats spectroscopically connect to the mechanistic function of natural light-harvesting?…”

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confidence: 99%

Vibronic mixing enables ultrafast energy flow in light-harvesting complex II

et al. 2020

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Since the discovery of quantum beats in the two-dimensional electronic spectra of photosynthetic pigment-protein complexes over a decade ago, the origin and mechanistic function of these beats in photosynthetic light-harvesting has been extensively debated. The current consensus is that these long-lived oscillatory features likely result from electronic-vibrational mixing, however, it remains uncertain if such mixing significantly influences energy transport. Here, we examine the interplay between the electronic and nuclear degrees of freedom (DoF) during the excitation energy transfer (EET) dynamics of light-harvesting complex II (LHCII) with two-dimensional electronic-vibrational spectroscopy. Particularly, we show the involvement of the nuclear DoF during EET through the participation of higher-lying vibronic chlorophyll states and assign observed oscillatory features to specific EET pathways, demonstrating a significant step in mapping evolution from energy to physical space. These frequencies correspond to known vibrational modes of chlorophyll, suggesting that electronic-vibrational mixing facilitates rapid EET over moderately size energy gaps.

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confidence: 99%

Vibronic mixing enables ultrafast energy flow in light-harvesting complex II

et al. 2020

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“…Traditionally this problem was addressed with the "core-system" approach. [1][2][3][4][5][6] This is to divide the overall environment into the "first-shell" and "secondary" parts. The core-system comprises both the primary system and the first-shell hybrid bath solvation modes.…”

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confidence: 99%

“…Various approximate theories such as quantum master equations had been applied to treat the reduced core-system dynamics under the influence of the secondary bath environments. [1][2][3][4][5][6] As exact methods are concerned, one often exploits the hierarchical-equations-of-motion (HEOM) formalism. 7-12 This is the time-derivative equivalence to the Feynman-Vernon influence functional path integral formalism, 13 which is exact for arbitrary systems coupling with Gaussian environments.…”

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confidence: 99%

Entangled system-and-environment dynamics: Phase–space dissipaton theory

Wang

Yan

2020

The Journal of Chemical Physics

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Dissipaton-equation-of-motion (DEOM) theory [Y. J. Yan, J. Chem. Phys. 140, 054105 (2014)] is an exact and nonperturbative many-particle method for open quantum systems. The existing dissipaton algebra treats also the dynamics of hybrid bath solvation coordinates. The dynamics of conjugate momentums remain to be addressed within the DEOM framework. In this work, we establish this missing ingredient, the dissipaton algebra on solvation momentums, with rigorous validations against necessary and sufficient criteria. The resulted phase-space DEOM theory will serve as a solid ground for further developments of various practical methods toward a broad range of applications. We illustrate this novel dissipaton algebra with the phase-space DEOM-evaluation on heat current fluctuation.

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“…Dynamical variables in DEOM are the dissipaton density operators (DDOs), for both the reduced system and and the hybrid bath dynamics. 10,11 The latter could also be measured experimentally, via such as the Fano interference, [12][13][14][15][16] vibronic spectroscopy with non-Condon polarized environment, 17 and transport current noise spectrum. 18 Dissipaton algebra plays essential roles here.…”

Section: Introductionmentioning

confidence: 99%

“…This noval algebra leads to the rules on how the DDOs evolves in time, and further on their relations to experimental measurable quantities that involve explicitly the hybrid bath dynamics. [14][15][16][17][18] From the algebraic construction point of view, the new DEOM theory in quest for amounts to the establishment of the generalized Wick's theorem with dissipatons-pairs added. This will be the new ingredient of the dissipaton algebra for treating the quadratic bath coupling in study.…”

Section: Introductionmentioning

confidence: 99%

Theory of Quantum Dissipation in a Class of Non-Gaussian Environments

Xu¹,

Liu²,

Zhang³

et al. 2017

Chinese Journal of Chemical Physics

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In this work we construct a novel dissipaton-equation-of-motion (DEOM) theory in quadratic bath coupling environment, based an extended algebraic statistical quasi-particle approach. To validate the new ingredient of the underlying dissipaton algebra, we derive an extended Zusman equation via a totally different approach. We prove that the new theory, if it starts with the identical setup, constitutes the dynamical resolutions to the extended Zusman equation. Thus, we verify the generalized (non-Gaussian) Wick's theorem with dissipatons-pair added. This new algebraic ingredient enables the dissipaton approach being naturally extended to nonlinear coupling environments. Moreover, it is noticed that, unlike the linear bath coupling case, the influence of a non-Gaussian environment cannot be completely characterized with the linear response theory. The new theory has to take this fact into account. The developed DEOM theory manifests the dynamical interplay between dissipatons and nonlinear bath coupling descriptors that will be specified. Numerical demonstrations will be given with the optical line shapes in quadratic coupling environment.

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Effects of Herzberg–Teller vibronic coupling on coherent excitation energy transfer

Cited by 43 publications

References 64 publications

Vibronic mixing enables ultrafast energy flow in light-harvesting complex II

Vibronic mixing enables ultrafast energy flow in light-harvesting complex II

Entangled system-and-environment dynamics: Phase–space dissipaton theory

Theory of Quantum Dissipation in a Class of Non-Gaussian Environments

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