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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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Organic solar cells are a promising route towards large‐area and low‐price photovoltaic systems. The devices are composed of at least two layers: the hole‐transport layer and the electron‐transport layer. The light absorption can occur in one or both layers. At the interface of the layers the excitons are separated into charge carriers, and every layer deals with one type of carrier. Higher efficiencies of the separation process can be obtained by using a mixed layer containing both materials to obtain a very high interface area. Although the structure of the mixed layers used plays a crucial role for the device performance, until now the morphologies have not been elucidated. In order to correlate physical and optical findings with structure and morphology for the materials in question, electron microscopy experiments were performed on the single components as well as on the layer systems. The conventional electron microscope is a poor phase microscope. As consequence, weak‐phase objects like organic molecules have to be stained or imaged under strong defocus to produce an observable contrast. Artifacts caused by chemical staining and the appearance of Fresnel diffraction using the defocus technique represent the main problems of conventional microscopy. These artifacts can be avoided using electron holography. Holograms of ultrathin sections of thin layers composed of organic dye molecules were recorded. Subsequently, the phase images were reconstructed. In this manner, we succeeded in obtaining high‐contrast electron micrographs without applying staining or defocus. In addition, holograms of crystalline C60 and zinc phthalocyanine were successfully recorded. Holography has been shown to be a useful tool to image beam‐sensitive and weak‐phase objects without artifacts. 相似文献
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Steven D. Bull Simon W. Epstein Nadeam Mujtaba Edward D. Savory Juan A. Tamayo 《Tetrahedron》2006,62(33):7911-7925
Enolates of (S)-N,N′-bis-(p-methoxybenzyl)-3-iso-propylpiperazine-2,5-dione exhibit high levels of enantiodiscrimination in alkylations with (RS)-1-aryl-1-bromoethanes and (RS)-2-bromoesters, affording substituted diketopiperazines containing two new stereogenic centres in high de. Deprotection and hydrolysis of the resultant substituted diketopiperazines provides a route to the asymmetric synthesis of homochiral methyl 2-amino-3-aryl-butanoates and 3-methyl-aspartates in high de and ee. 相似文献
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