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251.
Sithole M. A. Sharpey Schafer J. F. Majola S. N. T. Bucher T. D. Dinoko T. R. S. Ntshangase S. S. Lawrie E. A. Khumalo N. A. Jongile S. Mdletshe L. Bark R. A. Erasmus N. Jones P. Kheswa B. V. Lawrie J. J. Makhathini L. Malatji K. L. Maqabuka B. Noncolela S. P. Ndayishimye J. Shirinda O. Zikhali B. R. Masiteng P. L. 《The European Physical Journal A - Hadrons and Nuclei》2019,55(10):1-52
The European Physical Journal A - Photon strength functions describing the average response of the nucleus to an electromagnetic probe are key input information in the theoretical modelling of... 相似文献
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Chemically and Electrochemically Triggered Assembly of Viologen Radicals: Towards Multiaddressable Molecular Switches
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Christophe Kahlfuss Dr. Estelle Métay Marie‐Christine Duclos Prof. Marc Lemaire Prof. Anne Milet Prof. Eric Saint‐Aman Dr. Christophe Bucher 《Chemistry (Weinheim an der Bergstrasse, Germany)》2015,21(5):2090-2106
We have established that bipyridinium radicals can be reversibly π‐dimerized under the combined effects of chemical (proton transfer) and electrochemical (electron transfer) stimuli. Our investigations also led to the discovery that a bis‐pyridinyl appended calixarene intermediate is involved in a fully reversible redox‐triggered σ‐dimerization process. The structure of the most stable intramolecular σ‐dimer was provided by computational chemistry and its complete conversion into a noncovalent π‐dimer could be triggered chemically by addition of protons, leading to the formation of protonated cation radicals. Theoretical data collected with the N‐methylated and N‐protonated π‐dimers also support the existence of multivariant orientations in π‐bonded dimers of viologen cation‐radicals. 相似文献
255.
Dominik B. Bucher Alexander Schlueter Prof. Dr. Thomas Carell Prof. Dr. Wolfgang Zinth 《Angewandte Chemie (International ed. in English)》2014,53(42):11366-11369
Excited‐state dynamics are essential to understanding the formation of DNA lesions induced by UV light. By using femtosecond IR spectroscopy, it was possible to determine the lifetimes of the excited states of all four bases in the double‐stranded environment of natural DNA. After UV excitation of the DNA duplex, we detected a concerted decay of base pairs connected by Watson–Crick hydrogen bonds. A comparison of single‐ and double‐stranded DNA showed that the reactive charge‐transfer states formed in the single strands are suppressed by base pairing in the duplex. The strong influence of the Watson–Crick hydrogen bonds indicates that proton transfer opens an efficient decay path in the duplex that prohibits the formation or reduces the lifetime of reactive charge‐transfer states. 相似文献
256.
Fingerprinting DNA Oxidation Processes: IR Characterization of the 5‐Methyl‐2′‐Deoxycytidine Radical Cation
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Dominik B. Bucher Bert M. Pilles Toni Pfaffeneder Prof. Dr. Thomas Carell Prof. Wolfgang Zinth 《Chemphyschem》2014,15(3):420-423
Methylated cytidine plays an important role as an epigenetic signal in gene regulation. Its oxidation products are assumed to be involved in active demethylation processes but also in damaging DNA. Here, we report the photochemical production of the 5‐methyl‐2′‐deoxycytidine radical cation via a two‐photon ionization process. The radical cation is detected by time‐resolved IR spectroscopy and identified by band assignment using density functional theory calculations. Two final oxidation products are characterized with liquid chromatography coupled to mass spectrometry. 相似文献
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—This paper presents a new numerical code for determining the reliability of multi- degree-of-freedom (MDOF) linear or non-linear models of structure Several examples of application are presented. They are discussed in context with the issue of accuracy and computational efficiency of the new code and of other approximate solution methods such as statistical linearization. 相似文献
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Naitabdi A Toulemonde O Bucher JP Rosé J Braunstein P Welter R Drillon M 《Chemistry (Weinheim an der Bergstrasse, Germany)》2008,14(8):2355-2362
The controlled stoichiometry of heterometallic carbonyl clusters make them attractive precursors for the stabilization of bare metal alloy clusters for magnetic applications. The mixed-metal molecular cluster [RuCo3(H)(CO)12] has been functionalized with the phosphane-thiol ligand Ph2PCH2CH2SH to allow subsequent anchoring on a gold surface. The resulting tetrahedral cluster [RuCo3(H)(CO)11(Ph2PCH2CH2SH)] (1) has been characterized by X-ray diffraction and the P-monodentate ligand is axially bound to a cobalt center and trans to the ruthenium cap. This synthesis also yielded the product of oxidative coupling, in which two SH groups were coupled intermolecularly to give a disulfide ligand that links two tetrahedral cluster units in [{RuCo3(H)(CO)11(Ph2PCH2CH2S)}2] (2). This cluster has also been characterized by X-ray diffractions studies. After deposition of 1 on a Au(111) surface by self-assembly, the carbonyl ligands were stripped off by thermal annealing in ultra-high vacuum (UHV) to form a metallic species. X-ray photoelectron spectroscopic measurements performed as a function of the annealing temperature show that the cobalt and ruthenium centers converge towards metallic character and that the stoichiometry of the alloy is retained during the annealing process. Preliminary X-ray absorption spectroscopy (XAS) synchrotron experiments indicate that clusters 1 and 2 behave similarly, which is consistent with the retention of their tetrahedral units on the gold surface after transformation of the thiol function or breaking of the disulfide bond to form Au--S bonds, respectively, has occurred. 相似文献
259.
A series of enyne-allenes, with and without benzannulation at the ene moiety and equipped with aromatic and carbonyl groups as internal triplet sensitizer units at the allene terminus, was synthesized. Both sets, the cyclohexenyne-allenes and benzenyne-allenes, underwent thermal C(2)-C(6) cyclization exclusively to formal ene products. In contrast, the photochemical C(2)-C(6) cyclization of enyne-allenes provided formal Diels-Alder and/or ene products, with higher yields for the benzannulated systems. A raise of the temperature in the photochemical cyclization of enyne-allene 1b' led to increasing amounts of the ene product in relation to that of the formal Diels-Alder product. Laser flash photolysis at 266 and 355 nm as well as triplet quenching studies for 1b,b' indicated that the C(2)-C(6) cyclization proceeds via the triplet manifold. On the basis of a density functional theory (DFT) study, a short-lived transient (tau = 30 ns) was assigned as a triplet allene, while a long-lived transient (tau = 33 micros) insensitive to oxygen was assigned as fulvene triplet diradical. An elucidation of the reaction mechanism using extensive DFT computations allowed rationalization of the experimental product ratio and its temperature dependence. 相似文献
260.