Charge and Energy Transfer Dynamics in Molecular Systems

May, Volkhard; Kühn, Oliver

doi:10.1002/9783527633791

Cited by 857 publications

(866 citation statements)

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“…The model follows the standard Frenkel-exciton description of light-harvesting complexes within the single exciton manifold. 3 The Hamiltonian in the site basis denoted by |m (each Chl constitutes one site of the N-sites complex) is…”

Section: Modelling Exciton-dynamics In Lhc IImentioning

confidence: 99%

“…For light-harvesting complexes, usually these models are based on the Frenkel-exciton description. [1][2][3] With the availability of femto-second laser sources for triggering the excitation, a detailed, quantitative experimental study of the transport sequence has been achieved with time-resolved 2d-echo spectra and transient absorption spectra. The recorded 2d-echo spectra of the FennaMatthews-Olson (FMO) complex [4][5][6] and the light-harvesting complex II (LHC II) 7 contain a wealth of information and show the dissipative nature of the excitonic transport in form of the movement of peak intensity from the initially excited states along the diagonal of the 2d-spectra toward lower-energy, off-diagonal locations.…”

Section: Introductionmentioning

confidence: 99%

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Scalable High-Performance Algorithm for the Simulation of Exciton Dynamics. Application to the Light-Harvesting Complex II in the Presence of Resonant Vibrational Modes

Kreisbeck

Kramer

Aspuru‐Guzik

2014

J. Chem. Theory Comput.

120

160

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The accurate simulation of excitonic energy transfer in molecular complexes with coupled electronic and vibrational degrees of freedom is essential for comparing excitonic systemparameters obtained from ab-initio methods with measured time-resolved spectra. Several exact methods for computing the exciton dynamics within a density-matrix formalism are known, * To whom correspondence should be addressed † Institut für Physik, Humboldt-Universität zu Berlin, Newtonstr. 15, 12489 Berlin, Germany ‡ Mads Clausen Institute, University of Southern Denmark, Alsion 2, 6400 Sønderborg, Denmark ¶ Department of Chemistry and Chemical Biology, Harvard University, 12 Oxford St, Cambridge, Massachusetts 02138, USA 1 but are restricted to small systems with less than ten sites due to their computational complexity. To study the excitonic energy transfer in larger systems, we adapt and extend the exact hierarchical equation of motion (HEOM) method to various high-performance many-core platforms using the Open Compute Language (OpenCL). For the light-harvesting complex II (LHC II) found in spinach, the HEOM results deviate from predictions of approximate theories and clarify the time-scale of the transfer-process. We investigate the impact of resonantly coupled vibrations on the relaxation and show that the transfer does not rely on a fine-tuning of specific modes.

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Section: Modelling Exciton-dynamics In Lhc IImentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Scalable High-Performance Algorithm for the Simulation of Exciton Dynamics. Application to the Light-Harvesting Complex II in the Presence of Resonant Vibrational Modes

Kreisbeck

Kramer

Aspuru‐Guzik

2014

J. Chem. Theory Comput.

120

160

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“…If we treat the nuclear degrees of freedom classically, the wave function of the exciton system is described with the time-dependent Schrödinger equation [46]:…”

Section: Theorymentioning

confidence: 99%

Theoretical characterization of excitation energy transfer in chlorosome light-harvesting antennae from green sulfur bacteria

et al. 2014

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We present a theoretical study of excitation dynamics in the chlorosome antenna complex of green photosynthetic bacteria based on a recently proposed model for the molecular assembly. Our model for the excitation energy transfer (EET) throughout the antenna combines a stochastic time propagation of the excitonic wave function with molecular dynamics simulations of the supramolecular structure, and electronic structure calculations of the excited states. We characterized the optical properties of the chlorosome with absorption, circular dichroism and fluorescence polarization anisotropy decay spectra. The simulation results for the excitation dynamics reveal a detailed picture of the EET in the chlorosome. Coherent energy transfer is significant only for the first 50 fs after the initial excitation, and the wavelike motion of the exciton is completely damped at 100 fs. Characteristic time constants of incoherent energy transfer, subsequently, vary from 1 ps to several tens of ps. We assign the time scales of the EET to specific physical processes by comparing our results with the data obtained from time-resolved spectroscopy experiments.

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“…A systematic approach to derive a ME from a microscopic model is given by the Nakajima-Zwanzig projection operator method. [71][72][73][74] Alternatively, phenomenological approaches are also often advocated. A popular form of Markovian ME which is often used in the literature is the generalized Kossakowski-Lindblad (KL) equation: [75][76][77] …”

Section: Positivity Of the Kossakowski-lindblad Master Equation Irmentioning

confidence: 99%

Remarks on time-dependent [current]-density functional theory for open quantum systems

Yuen-Zhou

Aspuru‐Guzik

2013

Phys. Chem. Chem. Phys.

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Time-dependent [current]-density functional theory for open quantum systems (OQS) has emerged as a formalism that can incorporate dissipative effects in the dynamics of many-body quantum systems.Here, we review and clarify some formal aspects of these theories that have been recently questioned in the literature. In particular, we provide theoretical support for the following conclusions: (1) contrary to what we and others had stated before, within the master equation framework, there is in fact a one-to-one mapping between vector potentials and current densities for fixed initial state, particleparticle interaction, and memory kernel; (2) regardless of the first conclusion, all of our recently suggested Kohn-Sham (KS) schemes to reproduce the current and particle densities of the original OQS, and in particular, the use of a KS closed driven system, remains formally valid; (3) the Lindblad master equation maintains the positivity of the density matrix regardless of the time-dependence of the Hamiltonian or the dissipation operators; (4) within the stochastic Schrödinger equation picture, a one-to-one mapping from stochastic vector potential to stochastic current density for individual trajectories has not been proven so far, except in the case where the vector potential is the same for every member of the ensemble, in which case, it reduces to the Lindblad master equation picture; (5) master equations may violate certain desired properties of the density matrix, such as positivity, but they remain as one of the most useful constructs to study OQS when the environment is not easily incorporated explicitly in the calculation. The conclusions support our previous work as formally rigorous, offer new insights into it, and provide a common ground to discuss related theories.

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Charge and Energy Transfer Dynamics in Molecular Systems

Cited by 857 publications

References 0 publications

Scalable High-Performance Algorithm for the Simulation of Exciton Dynamics. Application to the Light-Harvesting Complex II in the Presence of Resonant Vibrational Modes

Scalable High-Performance Algorithm for the Simulation of Exciton Dynamics. Application to the Light-Harvesting Complex II in the Presence of Resonant Vibrational Modes

Theoretical characterization of excitation energy transfer in chlorosome light-harvesting antennae from green sulfur bacteria

Remarks on time-dependent [current]-density functional theory for open quantum systems

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