Linear and nonlinear optical responses in bacteriochlorophyll a

Sugisaki, Mitsuru; Fujii, Ritsuko; Cogdell, Richard J.; Hashimoto, Hideki

doi:10.1007/s11120-007-9266-x

Cited by 9 publications

(7 citation statements)

References 54 publications

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“…Bacteriochlorophyll (BChl) a (Figure ) plays important roles in efficient energy transfer of photosynthetic systems as energy carriers in light-harvesting antennas such as Fenna–Matthews–Olson (FMO) complex, light-harvesting complex 1 (LH1) and LH2. − Thus, the excited-state properties of BChl a not only in proteins − but also in solutions, ,− low-temperature glasses, ,,, and polymer films , have been experimentally studied for a long time.…”

Section: Introductionmentioning

confidence: 99%

Theoretical Study on Excited States of Bacteriochlorophyll a in Solutions with Density Functional Assessment

et al. 2014

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The excited-state properties of bacteriochlorophyll (BChl) a in triethylamine, 1-propanol, and methanol are investigated with the time-dependent density functional theory by using the quantum mechanical and molecular mechanical reweighting free energy self-consistant field method. It is found that no prevalent density functionals can reproduce the experimental excited-state properties, i.e., the absorption and reorganization energies, of BChl a in the solutions. The parameter μ in the range-separated hybrid functional is therefore optimized to reproduce the differences of the absorption energies in the solutions. We examine the origin of the differences of the absorption energies in the solutions and find that sensitive balance between contributions of structural changes and solute-solvent interactions determines the differences. The accurate description of the excitation with the density functional with the adjusted parameter is therefore essential to the understanding of the excited-state properties of BChl a in proteins and also the mechanism of the photosynthetic systems.

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Section: Introductionmentioning

confidence: 99%

Theoretical Study on Excited States of Bacteriochlorophyll a in Solutions with Density Functional Assessment

et al. 2014

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“…The ultrafast nonlinear responses of photosynthetic pigments have been described previously. 12,[14][15][16][17] In these studies pump-probe and transient grating ͑TG͒ spectroscopies have been widely used. 18 The most important advantage of the TG spectroscopy in comparison with the pump-probe technique is that the TG signal is background free since it is detected along the phase-matched direction of three pump pulses.…”

Section: Introductionmentioning

confidence: 99%

Comparison of transient grating signals from spheroidene in an organic solvent and in pigment-protein complexes fromRhodobacter sphaeroides2.4.1

et al. 2010

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The concurrent dynamics of the electronic excitation and vibronic oscillations of spheroidene have been investigated by means of the transient grating ͑TG͒ spectroscopy. The third-order optical responses of spheroidene in an organic solvent, in the LH2 light-harvesting antenna complexes, and in chromatophores have been compared in order to investigate the influence of the environment surrounding this photosynthetic pigment. Vibronic coherent oscillations with a period of several tens of femtosecond have been clearly observed superimposed on a slowly varying background, which reflects the electronic dynamics. The dynamics of the coherent oscillations have been analyzed by means of the wavelet analysis. Within our experimental accuracy, the decay times of the C v C and C u C stretching modes and C u CH 3 rocking mode of each specimen are very close. The experimental results have also been analyzed using a Brownian oscillator model. For these numerical calculations, the spectral density for the underdamped modes has been determined from the Raman spectrum of spheroidene. It was found that the low-frequency modes that reflect the influence of the protein environment can be approximated by the overdamped Brownian oscillator. The experimentally observed linear absorption spectra as well as the third-order optical responses, i.e., TG curves, are reproduced very well by these calculations. The close agreement between the experiments and calculations indicates that the Feynmandiagrammatic approach can be applied to express not only the internal conversion but also the intermolecular excitation energy-transfer processes. The vibronic decay rates of spheroidene in LH2 complexes and chromatophores are evaluated to be about 20% larger than in the organic solvent.

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“…The two lowest excited states designated as the Q x and Q y states play key roles in the primary stages of light-harvesting because they act as acceptors of energy transduction from carotenoids [11]. In contrast to the intensive studies of the Q y excited state dynamics of Bchl a [12][13][14][15][16], the dynamics of the Q x state has been poorly understood because of its extremely fast decay [17][18][19]. Previous studies have suggested that deactivation of the Q x state takes place in the range between 100~400 fs, while a detailed dynamics of the Q x state has not been sufficiently understood.…”

Section: Introductionmentioning

confidence: 99%

“…1(C)) was extracted from growth cells of Rhodobacter sphaeroides 2.4.1. Monomeric Bchl a was purified on a column of microcrystalline cellulose [12] and was dissolved in acetone. The absorbance was adjusted to 0.5 at excitation energy.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast excited state dynamics of monomeric bacteriochlorophyll a

Kosumi

Maruta

Fujii

et al. 2010

Phys. Status Solidi (c)

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Ultrafast excited state dynamics of the photosynthetic pigment bacteriochlorophyll a in solution have been investigated by means of steady‐state and time‐resolved spectroscopic techniques. Photo‐induced absorption spectra were observed upon excitation of bacteriochlorophyll a into its Qy or Qx absorption band. We show an incorporation of the Qx state in the ultrafast excited state dynamics of Bchl a in solution based on a comparison of transient absorption, beaching, and stimulated emission kinetics after excitation to the Qx or Qy band. (© 2011 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)

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Linear and nonlinear optical responses in bacteriochlorophyll a

Cited by 9 publications

References 54 publications

Theoretical Study on Excited States of Bacteriochlorophyll a in Solutions with Density Functional Assessment

Theoretical Study on Excited States of Bacteriochlorophyll a in Solutions with Density Functional Assessment

Comparison of transient grating signals from spheroidene in an organic solvent and in pigment-protein complexes fromRhodobacter sphaeroides2.4.1

Ultrafast excited state dynamics of monomeric bacteriochlorophyll a

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