Abstract:
:The stacking of the bacteriochlorophyll (BChl) c macrocycles and the role of water in forming an aggregate sheet, in chlorosome, were examined by means of (13)C NMR spectroscopy, the measurement of the X-ray diffraction pattern, and (25)Mg NMR spectroscopy. (1) The stacking of the macrocycles, i.e., weakly overlapped dimers forming displaced layers, was selected out of six different kinds of stacking so far identified in the aggregates of isomeric BChl c in solution and in the solid aggregate of an isomeric mixture of BChl c extracted from Chlorobium limicola. The selection was based on the comparison of the intermolecular (13)C...(13)C magnetic-dipole correlations with the nearest-neighbor carbon-to-carbon close contacts simulated for the above six different stackings. It has turned out that the stacking of the macrocycles in chlorosome is basically the same as that in the in vitro solid aggregate. (2) The crucial role of water in stabilizing the aggregate structure in chlorosome was shown by tracing the dehydration processes and by comparison with the solid aggregate using the X-ray diffraction pattern. Possible binding sites of water molecules were located, by structural simulation, based on the particular stacking structure. (3) The dimer-based stacking of the macrocycles was evidenced by (25)Mg NMR spectroscopy, which exhibited a pair of signals showing different quadrupole coupling, due to the presence or absence of a water molecule in the axial position.
journal_name
Biochemistryjournal_title
Biochemistryauthors
Kakitani Y,Koyama Y,Shimoikeda Y,Nakai T,Utsumi H,Shimizu T,Nagae Hdoi
10.1021/bi801651wsubject
Has Abstractpub_date
2009-01-13 00:00:00pages
74-86issue
1eissn
0006-2960issn
1520-4995pii
10.1021/bi801651wjournal_volume
48pub_type
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