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131.
132.
Patrick Homenya Markus Messerschmidt Muhammad Nawaz Tahir Victor Martinez Yajun Cheng Jochen S. Gutmann Michael Klein Stefan Jung Morris Wolff Reza Saadat Driss Nariaki Roman Bo?a G?star Klingelh?fer Wolfgang Tremel Franz Renz 《Hyperfine Interactions》2012,205(1-3):63-67
The nonanuclear coordination compound [MoIV{(CN)FeIII(3-methyl-saldptn)}8]Cl4 exhibits multiple spin transitions (3-methyl-saldptn = N,N′-bis(3′′-methyl-2′′-hydroxy-benzyliden)-1,7-diamino-4-azaheptane). This spin crossover cluster is bound via a self-assembled monolayer onto a two dimensional array gold surface. M?ssbauer spectroscopy indicates that the thermally and optically induced spin crossover of the compound is maintained. Thereby, the foundation for its potential practical application (e.g. in the field of information storage) was laid. 相似文献
133.
Nikolaus Umlauf Nadja Klein Achim Zeileis 《Journal of computational and graphical statistics》2018,27(3):612-627
Bayesian analysis provides a convenient setting for the estimation of complex generalized additive regression models (GAMs). Since computational power has tremendously increased in the past decade, it is now possible to tackle complicated inferential problems, for example, with Markov chain Monte Carlo simulation, on virtually any modern computer. This is one of the reasons why Bayesian methods have become increasingly popular, leading to a number of highly specialized and optimized estimation engines and with attention shifting from conditional mean models to probabilistic distributional models capturing location, scale, shape (and other aspects) of the response distribution. To embed many different approaches suggested in literature and software, a unified modeling architecture for distributional GAMs is established that exploits distributions, estimation techniques (posterior mode or posterior mean), and model terms (fixed, random, smooth, spatial,…). It is shown that within this framework implementing algorithms for complex regression problems, as well as the integration of already existing software, is relatively straightforward. The usefulness is emphasized with two complex and computationally demanding application case studies: a large daily precipitation climatology, as well as a Cox model for continuous time with space-time interactions. Supplementary material for this article is available online. 相似文献
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A review of measured breakdown properties in insulating films and of electronic theories of breakdown shows both theoretical and experimental inconsistencies. A theory is proposed in which electronic breakdown is caused by local chance events, such as a succession of avalanches at one spot. Successive avalanches sustain the growth of space charges, the local cathode field, and the avalanche rate. When the cathode field becomes large enough to make continuation of avalanching a certainty, instability with current runaway arises, causing breakdown. According to theory, breakdowns occur over a range of fields, their chance increasing very strongly with field; the breakdowns occur randomly in space and in time; the time to instability on a breakdown event decreases as some exponential function of increasing field; the breakdown field can both increase and decrease with temperature; it may be electrode dependent, and it decreases first rapidly and then more slowly with increasing film thickness. Observations made in a number of insulating films support the proposed theory. 相似文献
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137.
Craig M. Davis Megan F. Klein Kenneth T. Nicholson 《Phosphorus, sulfur, and silicon and the related elements》2013,188(3):659-664
Attempts were made to synthesize dinuclear Group 6 metal complexes of the arachno -octahydrotriborate anion. Specifically, the dimer [CpW(CO) 3 ] 2 (Cp = m 5 -C 5 H 5 ) was employed as the metal reagent. However, the formation of dinuclear metallaborane complexes did not ensue. Rather, clean, rapid, systematic borane-cage expansion was observed. The [B 3 H 8 ] m cluster was quantitatively converted to B 5 H 9 ,[B 9 H 14 ] m , or [B 11 H 14 ] m , or both, depending on reaction conditions. Refluxing a 1:1 mixture of [B 3 H 8 ] m and [CpW(CO) 3 ] 2 in toluene or dioxane lead to the rapid, quantitative conversion of [B 3 H 8 ] m to B 5 H 9 . However, refluxing a 2:1 mixture of [B 3 H 8 ] m and [CpW(CO) 3 ] 2 in the same solvents yielded [B 9 H 14 ] m and [B 11 H 14 ] m as the primary products; when glyme was the solvent, only [B 9 H 14 ] m was observed, even after prolonged heating. 相似文献
138.
Damir A. Safin Maria G. Babashkina Michael Bolte Axel Klein 《Phosphorus, sulfur, and silicon and the related elements》2013,188(12):2426-2432
The reaction of O,O′-diisopropylphosphoric acid isothiocyanate (iPrO)2P(O)NCS with 2-methylaniline 2-MeC6H4NH2, 2,6-dimethylaniline 2,6-Me2C6H3NH2, or 2,4,6-trimethylaniline 2,4,6-Me3C6H2NH2 leads to the N-phosphorylated thioureas RNHC(S)NHP(O)(OiPr)2 (R = 2-MeC6H4?, HLI ; 2,6-Me2C6H3?, HLII ; 2,4,6-Me3C6H2?, HLIII ). Reaction of the potassium salts of HLI –III with Ni(II) in aqueous EtOH leads to [Ni(LI–III-N,S)2] ([NiLI–III 2 ]) chelate complexes. The compounds obtained were investigated by 1H, 31P{1H} NMR spectroscopy and microanalysis. The molecular structure of the thiourea HLIII was elucidated by single crystal X-ray diffraction analysis. Single crystal X-ray diffraction studies showed that HLIII forms both intra- and intermolecular hydrogen bonds, which in turn leads to the formation of polymeric chains. One of the intermolecular hydrogen bonds is of the type N?H…S. Moreover, the formation of intermolecular C?H…η6-phenyl interactions was established. Supplemental materials are available for this article. Go to the publisher's online edition of Phosphorus, Sulfur, and Silicon and the Related Elements to view the free supplemental file. 相似文献
139.
J. C.T.R. Burckett St. Laurent P. B. Hitchcock M. A. King H. W. Kroto M. F. Meidine S. I. Klein 《Phosphorus, sulfur, and silicon and the related elements》2013,188(1-3):259-262
Abstract The chemistry of the novel phospha-alkenes RP[dbnd]CR'2, and phospha-alkynes, RC[tbnd]P, containing 2pπ-3pπ bonds is of current interest.1,2 Recent molecular orbital calculations,3,4 suggest that the highest occupied molecular orbital in CH2[dbnd]PH is of the π-type with the phosphorus lone pair ó-orbital only slightly more stable while the π? lumo orbital is relatively low lying. We now report He (I) photoelectron spectroscopic studies on a variety of RC[tbnd]P molecules5,6 which indicate that the homo is also of the π-type and the π-σ separation is much greater than that found in the analogous RC[tbnd]N systems. 相似文献
140.