Exciton Analysis in 2D Electronic Spectroscopy

Cho, Minhaeng; Vaswani, Harsha M.; Brixner, Tobias; Stenger, Jens; Fleming, Graham R.

doi:10.1021/jp050788d

Cited by 414 publications

(662 citation statements)

References 70 publications

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“…The second pathway features the excitonic wave packet starting from exciton 7, flowing through excitons 5 and/or 4, then passing through exciton 2 and finally to exciton 1. This result is similar to previous studies using another green sulfur bacteria species, Chlorobium tepidum [41]. The only major difference in this result is the starting exciton number from both pathways.…”

Section: Resultssupporting

confidence: 91%

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Simulated two-dimensional electronic spectroscopy of the eight-bacteriochlorophyll FMO complex

Yeh

Kais

2014

The Journal of Chemical Physics

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The Fenna-Matthews-Olson (FMO) protein-pigment complex acts as a molecular wire between the outer antenna system and the reaction center (RC); it is an important model system to study the excitonic energy transfer. Recent crystallographic studies report the existence of an additional (eighth) bacteriochlorophyll a (BChl a). To understand the functionality of this eighth BChl, we simulated the two-dimensional electronic spectra of both the 7-site (apo form) and the 8-site (holo form) variant of the FMO complex from green sulfur bacteria, Prosthecochloris aestuarii. By comparing the difference between the spectrum, it was found that the eighth BChl can affect two different excitonic energy transfer pathways, these being:(1) directly involve in the first pathway 6 → 3 → 1 of the apo form model by passing the excitonic energy to exciton 6; and (2) increase the excitonic wave function overlap between excitons 4 and 5 in the second pathway (7 → 4,5 → 2 → 1) and thus increase the possible downward sampling routes across the BChls. * Corresponding author, kais@purdue.edu 2

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Section: Resultssupporting

confidence: 91%

“…The only major difference in this result is the starting exciton number from both pathways. In the work of Cho et al [41], the two pathways they obtained are: 7 → 3 → 1 and 6 → 5,4 → 2 → 1, where in our case we find: 6 → 3 → 1 and 7…”

Section: Resultssupporting

confidence: 65%

Simulated two-dimensional electronic spectroscopy of the eight-bacteriochlorophyll FMO complex

Yeh

Kais

2014

The Journal of Chemical Physics

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“…For those systems, 2D electronic spectra provide detailed information on the electronic couplings among chromophores and on the excited energy and coherence transfer. [61][62][63][64][65] We leave them for future studies. Figure 3.…”

Section: Discussionmentioning

confidence: 99%

Dynamics of a Multimode System Coupled to Multiple Heat Baths Probed by Two-Dimensional Infrared Spectroscopy

2007

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Reduced equation of motion for a multimode system coupled to multiple heat baths is constructed by extending the quantum Fokker-Planck equation with low-temperature correction terms (J. Phys. Soc. Jpn. 2005, 74, 3131). Unlike such common approaches used to describe intramolecular multimode vibration as a BlochRedfield theory and a stochastic theory, the present formalism is defined by the molecular coordinates. To explore the correlation among different modes through baths, we consider two cases of system-bath couplings. One is a correlated case in which two modes are coupled to a single bath, and the other is an uncorrelated case in which each mode is coupled to a different bath. We further classify the correlated case into two cases, the plus-and minus-correlated cases, according to distinct correlation manners. For these, one-dimensional and two-dimensional infrared (2D-IR) spectra are calculated numerically by solving the equation of motion. It is demonstrated that 2D-IR spectroscopy has the ability to analyze the correlation of fluctuation-dissipation processes among different modes.

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“…Frenkel exciton model in conjugation with the Redfield equations, often in combination with the Förster theory, is behind a substantial part of the qualitative insight we have into the inner workings of photosynthesis (see e.g. [16,[20][21][22][23]). The two general theories described above are often stretched beyond their formal region of validity, even though they rarely cease to deliver meaningful physical insights.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast energy transfer with competing channels: Non-equilibrium Förster and Modified Redfield theories

Seibt

Mančal

2017

The Journal of Chemical Physics

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We derive equations of motion for the reduced density matrix of a molecular system which undergoes energy transfer dynamics competing with fast internal conversion channels. Environmental degrees of freedom of such a system have no time to relax to quasi-equilibrium in the electronic excited state of the donor molecule, and thus the conditions of validity of Förster and Modified Redfield theories in their standard formulations do not apply. We derive non-equilibrium versions of the two well-known rate theories and apply them to the case of carotenoid-chlorophyll energy transfer. Although our reduced density matrix approach does not account for the formation of vibronic excitons, it still confirms the important role of the donor ground-state vibrational states in establishing the resonance energy transfer conditions. We show that it is essential to work with a theory valid in strong system-bath interaction regime to obtain correct dependence of the rates on donor-acceptor energy gap.

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Exciton Analysis in 2D Electronic Spectroscopy

Cited by 414 publications

References 70 publications

Simulated two-dimensional electronic spectroscopy of the eight-bacteriochlorophyll FMO complex

Simulated two-dimensional electronic spectroscopy of the eight-bacteriochlorophyll FMO complex

Dynamics of a Multimode System Coupled to Multiple Heat Baths Probed by Two-Dimensional Infrared Spectroscopy

Ultrafast energy transfer with competing channels: Non-equilibrium Förster and Modified Redfield theories

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