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Linear and nonlinear optical responses in bacteriochlorophyll a

Photosynthesis Research volume 95, pages 309–316 (2008)Cite this article

Abstract

Nonlinear optical responses of bacteriochlorophyll a (BChl a) were investigated by means of the three-pulse four-wave mixing (FWM) technique under the resonant excitation into the Q y band. The experimental results are explained by a theoretical model calculation including the Brownian oscillation mode of the solvent. We have determined the spectral density, which is the most important function with which to calculate optical signals. The linear absorption spectrum can be reproduced fairly well when the vibronic oscillation modes of the solvent together with those of BChl a are properly taken into consideration. The FWM signal was also calculated using the spectral density. It was found that a simple two-level model could not explain the experimental result. The effect of the higher-order interactions is discussed.

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Abbreviations

BChl:

Bacteriochlorophyll

FWM:

Four-wave mixing

LH1:

Light-harvesting 1

LH2:

Light-harvesting 2

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Acknowledgments

The authors wish to thank Prof. Tadashi Mizoguchi and Prof. Hitoshi Tamiaki of Ritsumeikan University for valuable comments in preparing BChl a sample. This work was supported in part by the Grant-in-aid from the Japanese Ministry of Education, Culture, Sports, Science, and Technology (Grants No. 17204026, No. 17654083, No. 18340091, and No. 18654074). HH, MS, and RF thank for the financial support from SICP/JST. HH also acknowledges the support from PRESTO/JST.

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Affiliations

  1. Graduate School of Science, Osaka City University, Sugimoto, Sumiyoshi, Osaka, 558-8585, Japan

    Mitsuru Sugisaki, Ritsuko Fujii & Hideki Hashimoto

  2. Glasgow Biomedical Research Centre, IBLS, University of Glasgow, Glasgow, G12 8TA, Scotland, UK

    Richard J. Cogdell

Authors
  1. Mitsuru Sugisaki
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  2. Ritsuko Fujii
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  3. Richard J. Cogdell
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  4. Hideki Hashimoto
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Correspondence to Mitsuru Sugisaki.

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Sugisaki, M., Fujii, R., Cogdell, R.J. et al. Linear and nonlinear optical responses in bacteriochlorophyll a . Photosynth Res 95, 309–316 (2008). https://doi.org/10.1007/s11120-007-9266-x

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Keywords

  • Nonlinear spectroscopy
  • Four-wave mixing
  • BChl a
  • Brownian oscillator model
  • Spectral density