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1.
Laurens Kooijman Dr. Matthias Schuster Christian Baumann Simon Jurt Dr. Frank Löhr Dr. Boris Fürtig Prof. Dr. Peter Güntert Prof. Dr. Oliver Zerbe 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(47):21151-21158
To achieve efficient proton pumping in the light-driven proton pump bacteriorhodopsin (bR), the protein must be tightly coupled to the retinal to rapidly convert retinal isomerization into protein structural rearrangements. Methyl group dynamics of bR embedded in lipid nanodiscs were determined in the dark-adapted state, and were found to be mostly well ordered at the cytosolic side. Methyl groups in the M145A mutant of bR, which displays only 10 % residual proton pumping activity, are less well ordered, suggesting a link between side-chain dynamics on the cytosolic side of the bR cavity and proton pumping activity. In addition, slow conformational exchange, attributed to low frequency motions of aromatic rings, was indirectly observed for residues on the extracellular side of the bR cavity. This may be related to reorganization of the water network. These observations provide a detailed picture of previously undescribed equilibrium dynamics on different time scales for ground-state bR. 相似文献
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Abachi S Derrick M Kooijman P Musgrave B Price LE Repond J Sugano K Blockus D Brabson B Brom J Jung C Ogren H Rust DR Akerlof C Chapman J Errede D Ken MT Meyer DI Neal H Nitz D Thun R Tschirhart R Baringer P Bylsma BG DeBonte R Koltick D Low EH McIlwain RL Miller DH Ng CR Shibata EI 《Physical review D: Particles and fields》1989,40(3):902-905
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Abachi S Akerlof C Baringer P Blockus D Brabson B Brom J Bylsma BG Chapman J Cork B DeBonte R Derrick M Errede D Gan KK Jung C Ken MT Koltick D Kooijman P Loeffler FJ Loos JS Low EH McIlwain RL Meyer DI Miller DH Musgrave B Neal H Ng CR Nitz D Ogren H Paik HW Price LE Rangan LK Repond J Rust DR Shibata EI Sugano K Thun R Tschirhart R 《Physical review letters》1987,59(22):2519-2522
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Abachi S Baringer P Bylsma BG DeBonte R Koltick D Loeffler FJ Low EH McIlwain RL Miller DH Ng CR Rangan LK Shibata EI Derrick M Gan KK Kooijman P Loos JS Musgrave B Price LE Repond J Sugano K Weiss JM Wood DE Blockus D Brabson B Brom J Jung C Ogren H Rust DR Akerlof C Chapman J Errede D Kesten P Meyer DI Nitz D Seidl AA Thun R Willutzky M Cork B 《Physical review letters》1986,57(16):1990-1993
7.
ten Cate AT Kooijman H Spek AL Sijbesma RP Meijer EW 《Journal of the American Chemical Society》2004,126(12):3801-3808
Bifunctional 2-ureido-4[1H]-pyrimidinone (UPy) derivatives can form small cyclic oligomers as well as long supramolecular polymers in chloroform solutions using the quadruple hydrogen-bonding motif. Ring-chain equilibria of a set of supramolecular monomers containing methyl-substituted alkyl linkers between the hydrogen-bonding UPy moieties were investigated by (1)H NMR spectroscopy and viscometry. The data were characterized in terms of critical concentration (CC, denoting the onset of polymerization) and equilibrium cyclic dimer concentration (EDC, representing preorganization of the monomer toward selective formation of cyclic dimer). Methyl substituents in the monomer were found to promote conformations favorable for cyclic dimerization, leading to an increase in both the EDC and the CC with respect to unsubstituted monomer. Furthermore, we observed an odd-even effect in the CC and EDC with increasing length of the linker between the hydrogen-bonding units. The combined results allow tuning of the critical concentration over a broad range and offer detailed information on the correlation between monomer structure, conformation, and polymerizability which may provide new insights for the study and design of other ring-chain equilibria or helix-random coil transitions. 相似文献
8.
van Wijk AA Spaans A Uzunbajakava N Otto C de Groot HJ Lugtenburg J Buda F 《Journal of the American Chemical Society》2005,127(5):1438-1445
To resolve the molecular basis of the coloration mechanism of alpha-crustacyanin, we used (13)C-labeled astaxanthins as chromophores for solid-state (13)C NMR and resonance Raman spectroscopy of [6,6',7,7']-(13)C(4) alpha-crustacyanin and [8,8',9,9',10,10',11,11',20,20']-(13)C(10) alpha-crustacyanin. We complement the experimental data with time-dependent density functional theory calculations on several models based on the structural information available for beta-crustacyanin. The data rule out major changes and strong polarization effects in the ground-state electron density of astaxanthin upon binding to the protein. Conformational changes in the chromophore and hydrogen-bond interactions between the astaxanthin and the protein can account only for about one-third of the total bathochromic shift in alpha-crustacyanin. The exciton coupling due to the proximity of two astaxanthin chromophores is found to be large, suggesting that aggregation effects in the protein represent the primary source of the color change. 相似文献
9.
ten Cate AT Dankers PY Kooijman H Spek AL Sijbesma RP Meijer EW 《Journal of the American Chemical Society》2003,125(23):6860-6861
Homochiral hydrogen-bonded cyclic assemblies are formed in dilute solutions of racemic supramolecular polymers based on the quadruple hydrogen bonding 2-ureido-4[1H]-pyrimidinone unit, as observed by 1H NMR and SEC experiments. Preorganization of the monomers and the combined binding strength of the eight hydrogen bonds result in a very high stability of the cyclic aggregates with pronounced selectivity between homochiral and heterochiral cyclic species, usually only observed in crystalline or liquid crystalline phases. 相似文献
10.
Hirst AR Smith DK Feiters MC Geurts HP 《Chemistry (Weinheim an der Bergstrasse, Germany)》2004,10(23):5901-5910
The self-assembly of diaminododecane solubilised by four different stereoisomeric dendritic peptides to form gel-phase materials in toluene was investigated. The second generation dendritic peptides were based on D- and L-lysine building blocks, and each contained three chiral centres. By designing dendritic peptides in which the configurations of the chiral centres were modified, and applying them as gelator units, the assembly of stereoisomers could be investigated. In all cases, the self-assembly of gelator units resulted in macroscopic gelation. However, the degree of structuring was modulated by the stereoisomers employed, an effect which changed the morphology and macroscopic behavior of the self-assembled state. Enantiomeric (L,L,L or D,D,D) gelator units formed fibrous molecular assemblies, whilst the racemic gel (50 % L,L,L : 50 % D,D,D) formed a flat structure with a "woven" appearance. Gelator units based on L,D,D or D,L,L dendritic peptides also formed fibrous assemblies, but small-angle X-ray scattering indicated significant morphological differences were caused by the switch in chirality. Furthermore, the macroscopic stability of the gel was diminished when these peptides were compared with their L,L,L or D,D,D analogues. In this paper it is clearly shown that individual stereocentres, on the molecular level, are directly related to the helicity within the fibre. It is argued that the chirality controls the pattern of hydrogen bonding within the assembly, and hence determines the extent of fibre formation and the macroscopic gel strength. 相似文献