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Dr. Yasunori Toda Takayuki Yoshida Kaoru Arisue Prof. Dr. Kazuaki Fukushima Dr. Hiroyoshi Esaki Ayaka Kikuchi Prof. Dr. Hiroyuki Suga 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(41):10578-10582
Chiral Lewis acid-catalyzed asymmetric alcohol addition reactions to cyclic carbonyl ylides generated from N-(α-diazocarbonyl)-2-oxazolidinones featuring a dual catalytic system are reported. Construction of a chiral quaternary heteroatom-substituted carbon center was accomplished in which the unique heterobicycles were obtained in good yields with high stereoselection. The alcohol adducts were successfully converted to optically active oxazolidine-2,4-diones by hydrolysis. Mechanistic studies by DFT calculations revealed that alcohols could be activated by Lewis acids, enabling enantioselective protonation of the carbonyl ylides. 相似文献
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Nakayama T Kamachi T Jitsumori K Omi R Hirotsu K Esaki N Kurihara T Yoshizawa K 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(27):8392-8402
The high substrate specificity of fluoroacetate dehalogenase was explored by using crystallographic analysis, fluorescence spectroscopy, and theoretical computations. A crystal structure for the Asp104Ala mutant of the enzyme from Burkholderia sp. FA1 complexed with fluoroacetate was determined at 1.2 ? resolution. The orientation and conformation of bound fluoroacetate is different from those in the crystal structure of the corresponding Asp110Asn mutant of the enzyme from Rhodopseudomonas palustris CGA009 reported recently (J. Am. Chem. Soc. 2011, 133, 7461). The fluorescence of the tryptophan residues of the wild-type and Trp150Phe mutant enzymes from Burkholderia sp. FA1 incubated with fluoroacetate and chloroacetate was measured to gain information on the environment of the tryptophan residues. The environments of the tryptophan residues were found to be different between the fluoroacetate- and chloroacetate-bound enzymes; this would come from different binding modes of these two substrates in the active site. Docking simulations and QM/MM optimizations were performed to predict favorable conformations and orientations of the substrates. The F atom of the substrate is oriented toward Arg108 in the most stable enzyme-fluoroacetate complex. This is a stable but unreactive conformation, in which the small O-C-F angle is not suitable for the S(N)2 displacement of the F(-) ion. The cleavage of the C-F bond is initiated by the conformational change of the substrate to a near attack conformation (NAC) in the active site. The second lowest energy conformation is appropriate for NAC; the C-O distance and the O-C-F angle are reasonable for the S(N) 2 reaction. The activation energy is greatly reduced in this conformation because of three hydrogen bonds between the leaving F atom and surrounding amino acid residues. Chloroacetate cannot reach the reactive conformation, due to the longer C-Cl bond; this results in an increase of the activation energy despite the weaker C-Cl bond. 相似文献
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We have obtained spectra for the LO phonon mode by Raman scattering associated with surface quantization of the hole states in the depletion layer of highly doped n-type GaAs samples. When semi-transparent metal contacts are employed, the zone-center LO peak shifts to higher frequency due to plasmon-phonon interaction. The observed effects are not sensitive to the types of metal. The presence of the plasmon mode is thought to be due to the steady-state carrier injection from the incident laser light. The position of the peak is used to estimate the surface recombination rate of the excited electron-hole pairs. 相似文献
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P. Voisin C. Delalande G. Bastard M. Voos L.L. Chang A. Segmuller C.A. Chang L. Esaki 《Superlattices and Microstructures》1985,1(2):155-159
We present optical absorption experiments performed at low temperature in very high quality GaSbAlSb superlattices grown by MBE. The absorption spectra exhibit pronounced exciton peaks separated by absorption plateaus. The data are interpreted within an effective mass theory, taking into account the effect of strains induced by the 0.65 % lattice mismatch of the hosts. From the number of observed transitions, we can determine quite accurately the band offsets in this system. The crossover of the quantized states originating from the Λ and L minima of the GaSb conduction band is also discussed. 相似文献
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[reaction: see text] A general and in situ D2 gas generation method using 10% Pd/C-catalyzed H2-D2 exchange reaction in a H2-D2O system has been developed. H2 gas sealed in a reaction flask was efficiently converted into nearly pure D2 gas, which can be used for the reductive deuteration of substrates possessing reducible functionalities within the molecule. 相似文献
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Toshiyuki Esaki 《Analytica chimica acta》1981,133(4):657-665
A graphic program for quantitative drug design is described; it is used for the design stage of candidate compounds after a regression equation has been established for estimation of biological potencies in the Hansch—Fujita and Free—Wilson methods. Information flow is controlled by function-key and concomitant alphanumeric-key operations. In the program, substituents are easily introduced into a parent structure, and a perspective molecular model of the resulting derivative is displayed. Conformational changes of a molecule can be followed by rotating atomic groups. The data bank contains 337 possible substituents with 20 physicochemical parameter values and constituent atomic coordinates for each substituent. Examples are shown to illustrate the program. 相似文献
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自然形成的岩石节理面的表面形状具有分形特性,利用分形理论来描述岩石节理的粗糙特性,并确立与岩石节理面的剪切力学特性间的关系对于指导岩体工程设计,和管理具有重要一研究利用开发设计的三维激光测距仪在精确测定岩石节理面的表面形状4 基础上,依据变量图法建立了 岩石节理面的 相似文献