Influence of phonons on exciton transfer dynamics: comparison of the Redfield, Förster, and modified Redfield equations

Yang, Mino; Fleming, Graham R.

doi:10.1016/s0301-0104(02)00604-3

Cited by 184 publications

(202 citation statements)

References 43 publications

Supporting

Mentioning

198

Contrasting

Order By: Relevance

“…27,32,[34][35][36][37] The combined Förster-Redfield theory requires an empirical parameter M cr for separating the exciton Hamiltonian between a strongly coupled part H strong ex with all off-diagonal elements set to zero except those |J mn | > M cr and the remaining weakly coupled sites. 58 Suggested values for LHC II are M cr = 20 cm −1 or smaller. 27,35 method is free of these restrictions and allows one to track the exciton-dynamics also through a network with the excitation emanating from a localized site.…”

Section: Influence Of the Vibrational Peaks On The Transport In Lhc IImentioning

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

View full text Add to dashboard Cite

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.

show abstract

Section: Influence Of the Vibrational Peaks On The Transport In Lhc IImentioning

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

View full text Add to dashboard Cite

show abstract

“…Recently, quantum-classical mixed methods have been also applied to the dynamics of energy transfer [28][29][30]. Different theoretical methods have been tested in the simple two-site system [11] and other complex systems [27], mainly focusing on the reliability of theoretical predictions.…”

Section: Introductionmentioning

confidence: 99%

Efficient energy transfer in light-harvesting systems: Quantum-classical comparison, flux network, and robustness analysis

Liu

et al. 2012

The Journal of Chemical Physics

102

137

View full text Add to dashboard Cite

Following the calculation of optimal energy transfer in thermal environment in our first paper (Wu et al., New J. Phys., 2010, 12, 105012), full quantum dynamics and leading-order 'classical' hopping kinetics are compared in the seven-site Fenna-Matthews-Olson (FMO) protein complex.The difference between these two dynamic descriptions is due to higher-order quantum corrections.Two thermal bath models, classical white noise (the Haken-Strobl-Reineker model) and quantum Debye model, are considered. In the seven-site FMO model, we observe that higher-order corrections lead to negligible changes in the trapping time or in energy transfer efficiency around the optimal and physiological conditions (2% in the HSR model and 0.1% in the quantum Debye model for the initial site at BChl 1). However, using the concept of integrated flux, we can identify The eight-site FMO model yields similar trapping time and network structure as the seven-site FMO model but leads to a more disperse distribution of energy transfer pathways.2

show abstract

“…Such work has sought to explain the origin of the observed coherence lifetime, to predict the effects of system parameters, and to ultimately understand the role of quantum coherence in promoting or inhibiting efficient energy transfer. [5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20][21] EET systems typically consist of a set of molecular chromophores which are electronically coupled to one another as well as to local environmental phonons. The former couplings facilitate exciton delocalization while the latter couplings tend to destroy this so-called quantum coherence.…”

Section: Introductionmentioning

confidence: 99%

Reduced density matrix hybrid approach: Application to electronic energy transfer

Berkelbach

Markland

Reichman

2012

The Journal of Chemical Physics

View full text Add to dashboard Cite

Electronic energy transfer in the condensed phase, such as that occurring in photosynthetic complexes, frequently occurs in regimes where the energy scales of the system and environment are similar. This situation provides a challenge to theoretical investigation since most approaches are accurate only when a certain energetic parameter is small compared to others in the problem. Here we show that in these difficult regimes, the Ehrenfest approach provides a good starting point for a dynamical description of the energy transfer process due to its ability to accurately treat coupling to slow environmental modes. To further improve on the accuracy of the Ehrenfest approach, we use our reduced density matrix hybrid framework to treat the faster environmental modes quantum mechanically, at the level of a perturbative master equation. This combined approach is shown to provide an efficient and quantitative description of electronic energy transfer in a model dimer and the Fenna-Matthews-Olson complex and is used to investigate the effect of environmental preparation on the resulting dynamics.

show abstract

Influence of phonons on exciton transfer dynamics: comparison of the Redfield, Förster, and modified Redfield equations

Cited by 184 publications

References 43 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

Efficient energy transfer in light-harvesting systems: Quantum-classical comparison, flux network, and robustness analysis

Reduced density matrix hybrid approach: Application to electronic energy transfer

Contact Info

Product

Resources

About