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Circular dichroism and resonance Raman spectroscopies of bacteriochlorophyll b-containing LH1-RC complexes

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Abstract

The core light-harvesting complexes (LH1) in bacteriochlorophyll (BChl) b-containing purple phototrophic bacteria are characterized by a near-infrared absorption maximum around 1010 nm. The determinative cause for this ultra-redshift remains unclear. Here, we present results of circular dichroism (CD) and resonance Raman measurements on the purified LH1 complexes in a reaction center-associated form from a mesophilic and a thermophilic Blastochloris species. Both the LH1 complexes displayed purely positive CD signals for their Qy transitions, in contrast to those of BChl a-containing LH1 complexes. This may reflect differences in the conjugation system of the bacteriochlorin between BChl b and BChl a and/or the differences in the pigment organization between the BChl b- and BChl a-containing LH1 complexes. Resonance Raman spectroscopy revealed remarkably large redshifts of the Raman bands for the BChl b C3-acetyl group, indicating unusually strong hydrogen bonds formed with LH1 polypeptides, results that were verified by a published structure. A linear correlation was found between the redshift of the Raman band for the BChl C3-acetyl group and the change in LH1-Qy transition for all native BChl a- and BChl b-containing LH1 complexes examined. The strong hydrogen bonding and π–π interactions between BChl b and nearby aromatic residues in the LH1 polypeptides, along with the CD results, provide crucial insights into the spectral and structural origins for the ultra-redshift of the long-wavelength absorption maximum of BChl b-containing phototrophs.

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Abbreviations

Alc :

Allochromatium

BChl:

Bacteriochlorophyll

Blc :

Blastochloris

CD:

Circular dichroism

DDM:

n-dodecyl β-D-maltopyranoside

FWHM:

Full width at half maximum

Hlr :

Halorhodospira

LH:

Light-harvesting

RC:

Reaction center

Tch :

Thermochromatium

Trv :

Thiorhodovibrio

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Acknowledgements

We thank Ms. Madoka Yamashita of Kindai University for her experimental assistance, JASCO Corporation (Japan) for measurements of CD spectra, Ms. Satoko Suzuki, Mr. Yoshiro Kondo and Ms. Miwako Kobayashi of JASCO Corporation for assistance in CD measurements, Kao Corporation for providing detergent LDAO. This work was supported in part by Grants-in-aid for Scientific Research (C) (19K06563) to Y.K., JSPS KAKENHI Grant Numbers JP16H04174, JP18H05153, JP20H05086 and JP20H02856, Takeda Science Foundation, the Kurata Memorial Hitachi Science and Technology Foundation, Japan to Z.-Y.W.-O. and the National Key R&D Program of China (No. 2019YFA0904600) to L.-J. Y.

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Authors and Affiliations

  1. Department of Agrobioscience, Graduate School of Agriculture, Kobe University, Nada, Kobe, 657-8501, Japan

    Y. Kimura, R. Seto, M. Imanishi & S. Takenaka

  2. Faculty of Science, Ibaraki University, Mito, 310-8512, Japan

    T. Yamashita, M. Honda & Z.-Y. Wang-Otomo

  3. Department of Chemistry, Kindai University, Higashi-Osaka, 577-8502, Japan

    S. Nakagawa & Y. Saga

  4. Photosynthesis Research Center, Key Laboratory of Photobiology, Institute of Botany, Chinese Academy of Sciences, Beijing, 100093, China

    L.-J. Yu

  5. Department of Microbiology, Southern Illinois University, Carbondale, IL, 62901, USA

    M. T. Madigan

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  1. Y. Kimura
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  2. T. Yamashita
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  4. M. Imanishi
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  11. Z.-Y. Wang-Otomo
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Correspondence to Y. Kimura or Z.-Y. Wang-Otomo.

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Kimura, Y., Yamashita, T., Seto, R. et al. Circular dichroism and resonance Raman spectroscopies of bacteriochlorophyll b-containing LH1-RC complexes. Photosynth Res 148, 77–86 (2021). https://doi.org/10.1007/s11120-021-00831-5

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