Photo-CIDNP MAS NMR in intact cells of Rhodobacter sphaeroides R26: Molecular and atomic resolution at nanomolar concentration

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作者：
Prakash, Shipra [1 ]
Alia [1 ]
Gast, Peter [2 ]
De Groot, Huub J. M. [1 ]
Matysik, Jörg [1 ]
Jeschke, Gunnar [3 ]
机构：
[1] Leiden Institute of Chemistry, P.O. Box 9502, 2300 RA Leiden, Netherlands
[2] Leiden Institute of Physics, P.O. Box 9504, 2300 RA Leiden, Netherlands
[3] Department of Chemistry, University of Konstanz, 78457 Konstanz, Germany
来源：
Journal of the American Chemical Society | 2006年 / 128卷 / 39期
关键词：
Photochemically induced dynamic nuclear polarization (photo-CIDNP) is observed in photosynthetic reaction centers of the carotenoid-less strain R26 of the purple bacterium Rhodobacter sphaeroides by 13C solid-state NMR at three different magnetic fields (4.7; 9.4; and 17.6 T). The signals of the donor appear enhanced absorptive (positive) and of the acceptor emissive (negative). This spectral feature is in contrast to photo-CIDNP data of reactions centers of Rhodobacter sphaeroides wildtype reported previously (Prakash; S; Alia; Gast; P; de Groot; H; J; M; Jeschke; G; Matysik; Am; Chem; Soc; 2005; 127; 14290-14298) in which all signals appear emissive. The difference is due to an additional mechanism occurring in RCs of R26 in the long-living triplet state of the donor; allowing for spectral editing by different enhancement mechanisms. The overall shape of the spectra remains independent of the magnetic field. The strongest enhancement is observed at 4.7 T; enabling the observation of photo-CIDNP enhanced NMR signals from reaction center cofactors in entire bacterial cells allowing for detection of subtle changes in the electronic structure at nanomolar concentration of the donor cofactor. Therefore; we establish in this paper photo-CIDNP MAS NMR as a method to study the electronic structure of photosynthetic cofactors at the molecular and atomic resolution as well as at cellular concentrations. © 2006 American Chemical Society;
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页码：12794 / 12799
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