Application of the density matrix method to spectroscopy and dynamics of photosynthetic reaction centers

Hayashi, M.; Yang, Tsun-Hua; Chang, Chih-Yung; Liang, Ke; Chang, Rong‐Yeu; Lin, Sheng Hsien

doi:10.1002/1097-461x(2000)80:4/5<1043::aid-qua53>3.0.co;2-e

Cited by 7 publications

(1 citation statement)

References 69 publications

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“…The density matrix was propagated with time at 80 K by Runge–Kutta integration of the stochastic Liouville equation, including terms for coherence transfer and vibrational relaxations. ,,− The time constant for thermal equilibration of the two lowest levels of each vibrational mode was taken to be 2.0 ps. Time constants for pure dephasing due to vibrational and electronic inhomogeneity were set at 100 ps (too long for this process to affect the results).…”

Section: Methodsmentioning

confidence: 99%

Dynamics of the Excited State in Photosynthetic Bacterial Reaction Centers

Parson

2020

J. Phys. Chem. B

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In the initial charge-separation reaction of photosynthetic bacterial reaction centers, a dimer of strongly interacting bacteriochlorophylls (P) transfers an electron to a third bacteriochlorophyll (BL). It has been suggested that light first generates an exciton state of the dimer and that an electron then moves from one bacteriochlorophyll to the other within P to form a charge-transfer state (PL +PM –), which passes an electron to BL. This scheme, however, is at odds with the most economical analysis of the spectroscopic properties of the reaction center and particularly with the unusual temperature dependence of the long-wavelength absorption band. The present paper explores this conflict with the aid of a simple model in which exciton and charge-transfer states are coupled to three vibrational modes. It then uses a similar model to show that the main experimental evidence suggesting the formation of PL +PM – as an intermediate could reflect pure dephasing of vibrational modes that modulate stimulated emission.

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Section: Methodsmentioning

confidence: 99%

Dynamics of the Excited State in Photosynthetic Bacterial Reaction Centers

Parson

2020

J. Phys. Chem. B

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Theories and Quantum Chemical Calculations of Linear and Sum‐Frequency Generation Spectroscopies, and Intramolecular Vibrational Redistribution and Density Matrix Treatment of Ultrafast Dynamics

Yang

Niu²,

Lin

et al. 2014

Advances in Chemical Physics

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The First Picoseconds in Bacterial Photosynthesis—Ultrafast Electron Transfer for the Efficient Conversion of Light Energy

2005

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In this Minireview, we describe the function of the bacterial reaction centre (RC) as the central photosynthetic energy-conversion unit by ultrafast spectroscopy combined with structural analysis, site-directed mutagenesis, pigment exchange and theoretical modelling. We show that primary energy conversion is a stepwise process in which an electron is transferred via neighbouring chromophores of the RC. A well-defined chromophore arrangement in a rigid protein matrix, combined with optimised energetics of the different electron carriers, allows a highly efficient charge-separation process. The individual molecular reactions at room temperature are well described by conventional electron-transfer theory.

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Application of the density matrix method to spectroscopy and dynamics of photosynthetic reaction centers

Cited by 7 publications

References 69 publications

Dynamics of the Excited State in Photosynthetic Bacterial Reaction Centers

Dynamics of the Excited State in Photosynthetic Bacterial Reaction Centers

Theories and Quantum Chemical Calculations of Linear and Sum‐Frequency Generation Spectroscopies, and Intramolecular Vibrational Redistribution and Density Matrix Treatment of Ultrafast Dynamics

The First Picoseconds in Bacterial Photosynthesis—Ultrafast Electron Transfer for the Efficient Conversion of Light Energy

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