Magic-angle spinning nuclear magnetic resonance under ultrahigh field reveals two forms of intermolecular interaction within CH2Cl2-treated (31R)-type bacteriochlorophyll c solid aggregate

被引:19
作者
Umetsu, M
Hollander, JG
Matysik, J
Wang, ZY
Adschiri, T
Nozawa, T
de Groot, HJM
机构
[1] Leiden Univ, Leiden Inst Chem, Gorlaeus Labs, NL-2300 RA Leiden, Netherlands
[2] Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Aoba Ku, Sendai, Miyagi 9808577, Japan
[3] Tohoku Univ, Dept Biomol Engn, Grad Sch Engn, Aoba Ku, Sendai, Miyagi 9808579, Japan
关键词
D O I
10.1021/jp034957a
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
(3(1)R)-bacteriochlorophyll (BChl) c solid aggregates with an absorbance around 740 nm were formed from BChl c dimers, and 2-D homonuclear C-13-C-13 radio frequency-driven dipolar recoupling as well as proton-driven spin diffusion dipolar correlation NMR spectra have been collected in ultrahigh magnetic field. Doubling of signals is observed for most carbons in the BChl c macrocycle, leading to two correlation networks. In this way, two major fractions denoted types A and B are identified. Some of the ring carbons show multiple resonances, revealing additional slight differences in microstructural environment. 2-D heteronuclear H-1-C-13 correlation data have been recorded using the frequency- and phase-switched Lee-Goldburg technique to assign the H-1 response. N-15 chemical shifts are assigned from 2-D heteronuclear N-15-C-13 correlation experiments using spectrally induced filtering in combination with cross polarization. Also the nitrogen atoms in the pyrrole rings I, II, and IV (N-I, N-II, and N-IV, respectively) show two sets of resonances, each of which is connected to a single C-13 correlation network A or B. The C-13 chemical shifts are compared with the signals from antiparallel dimers in solution and with the response from chlorosomes previously reported. The data clearly show that the stacking in CH2Cl2-treated aggregates is different from the stacking in the chlorosomes and hexane-treated aggregates. Some degree of similarity with the antiparallel dimer form in solution transpires, in particular for the type A species. It is proposed that the CH2Cl2 precipitate represents a structural intermediate between the antiparallel dimer and the parallel stack as found in the chlorosome.
引用
收藏
页码:2726 / 2734
页数:9
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