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In connection with our synthetic approach to pentacyclic triterpenes,1 we have required substantial amounts of 2,5,5-trimethyl-1,3-cyclohexanedione (methyldimedone, 2), which is available by methylation of dimedone (1).2 However, methylation may also afford the 2,2-dimethyl product 3, the methyl ether 4, and the C, O-dimethyl product 5. 相似文献
66.
Susanne Kern Hafida Dkhil Prisca Hendarsa Graham Ellis Andreas Natsch 《Analytical and bioanalytical chemistry》2014,406(25):6165-6178
On prolonged exposure to air, linalool can form sensitizing hydroperoxides. Positive hydroperoxide patch tests in dermatitis patients have frequently been reported, but their relevance has not been established. Owing to a lack of analytical methods and data, it is unclear from which sources the public might be exposed to sufficient quantities of hydroperoxides for induction of sensitization to occur. To address this knowledge gap, we developed analytical methods and performed stability studies for fine fragrances and deodorants/antiperspirants. In parallel, products recalled from consumers were analysed to investigate exposure to products used in everyday life. Liquid chromatography–mass spectrometry with high mass resolution was found to be optimal for the selective and sensitive detection of the organic hydroperoxide in the complex product matrix. Linalool hydroperoxide was detected in natural linalool, but the amount was not elevated by storage in a perfume formulation exposed to air. No indication of hydroperoxide formation in fine fragrances was found in stability studies. Aged fine fragrances recalled from consumers contained a geometric mean linalool concentration of 1,888 μg/g and, corrected for matrix effects, linalool hydroperoxide at a concentration of around 14 μg/g. In antiperspirants, we detected no oxidation products. In conclusion, very low levels of linalool hydroperoxide in fragranced products may originate from raw materials, but we found no evidence for oxidation during storage of products. The levels detected are orders of magnitude below the levels inducing sensitization in experimental animals, and these results therefore do not substantiate a causal link between potential hydroperoxide formation in cosmetics and positive results of patch tests. Graphical Abstract
67.
Dr. Matthias Daxner Prof. Stephan Denifl Prof. Paul Scheier Prof. Andrew M. Ellis 《Angewandte Chemie (International ed. in English)》2014,53(49):13528-13531
The self‐assembly of salt nanocrystals from chemical reactions inside liquid helium is reported for the first time. Reaction is initiated by an electron impacting a helium nanodroplet containing sodium atoms and SF6 molecules, leading to preferential production of energetically favorable structures based on the unit cell of crystalline NaF. These favorable structures are observed as magic number ions (anomalously intense peaks) in mass spectra and are seen in both cationic and anionic channels in mass spectra, for example, (NaF)nNa+ and (NaF)nF?. In the case of anions the self‐assembly is not directly initiated by electrons: the dominant process involves resonant electron‐induced production of metastable electronically excited He? anions, which then initiate anionic chemistry by electron transfer. 相似文献
68.
Alba L. Montoya Eileni R. Gil Emily L. Heydemann Igor L. Estevao Bianca E. Luna Cameron C. Ellis Sohan R. Jankuru Belkisyol Alarcn de Noya Oscar Noya Maria Paola Zago Igor C. Almeida Katja Michael 《Molecules (Basel, Switzerland)》2022,27(2)
Chagas disease (CD) can be accurately diagnosed by detecting Trypanosoma cruzi in patients’ blood using polymerase chain reaction (PCR). However, parasite-derived biomarkers are of great interest for the serological diagnosis and early evaluation of chemotherapeutic efficacy when PCR may fail, owing to a blood parasite load below the method’s limit of detection. Previously, we focused on the detection of specific anti-α-galactopyranosyl (α-Gal) antibodies in chronic CD (CCD) patients elicited by α-Gal glycotopes copiously expressed on insect-derived and mammal-dwelling infective parasite stages. Nevertheless, these stages also abundantly express cell surface glycosylphosphatidylinositol (GPI)-anchored glycoproteins and glycoinositolphospholipids (GIPLs) bearing nonreducing terminal β-galactofuranosyl (β-Galf) residues, which are equally foreign to humans and, therefore, highly immunogenic. Here we report that CCD patients’ sera react specifically with synthetic β-Galf-containing glycans. We took a reversed immunoglycomics approach that entailed: (a) Synthesis of T. cruzi GIPL-derived Galfβ1,3Manpα-(CH2)3SH (glycan G29SH) and Galfβ1,3Manpα1,2-[Galfβ1,3]Manpα-(CH2)3SH (glycan G32SH); and (b) preparation of neoglycoproteins NGP29b and NGP32b, and their evaluation in a chemiluminescent immunoassay. Receiver-operating characteristic analysis revealed that NGP32b can distinguish CCD sera from sera of healthy individuals with 85.3% sensitivity and 100% specificity. This suggests that Galfβ1,3Manpα1,2-[Galfβ1,3]Manpα is an immunodominant glycotope and that NGP32b could potentially be used as a novel CCD biomarker. 相似文献
69.
Jean-Philippe Uzan George F. R. Ellis Julien Larena 《General Relativity and Gravitation》2011,43(1):191-205
In order to understand how locally static configurations around gravitationally bound bodies can be embedded in an expanding
universe, we investigate the solutions of general relativity describing a space–time whose spatial sections have the topology
of a 3-sphere with two identical masses at the poles. We show that Israel junction conditions imply that two spherically symmetric
static regions around the masses cannot be glued together. If one is interested in an exterior solution, this prevents the
geometry around the masses to be of the Schwarzschild type and leads to the introduction of a cosmological constant. The study
of the extension of the Kottler space–time shows that there exists a non-static solution consisting of two static regions
surrounding the masses that match a Kantowski–Sachs expanding region on the cosmological horizon. The comparison with a Swiss-Cheese
construction is also discussed. 相似文献
70.
The nature of the future is completely different from the nature of the past. When quantum effects are significant, the future
shows all the signs of quantum weirdness, including duality, uncertainty, and entanglement. With the passage of time, after
the time-irreversible process of state-vector reduction has taken place, the past emerges, with the previous quantum uncertainty
replaced by the classical certainty of definite particle identities and states. The present time is where this transition
largely takes place, but the process does not take place uniformly: evidence from delayed choice and related experiments shows
that isolated patches of quantum indeterminacy remain, and that their transition from probability to certainty only takes
place later. Thus, when quantum effects are significant, the picture of a classical Evolving Block Universe (‘EBU’) cedes
place to one of a Crystallizing Block Universe (‘CBU’), which reflects this quantum transition from indeterminacy to certainty,
while nevertheless resembling the EBU on large enough scales. 相似文献