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81.
The formation of Ni2O2 can be observed from the condensation of effusive beams of Ni and O2 in neon or argon matrices. Observation of 58Ni(2)16O2, 58Ni60Ni16O2, 60Ni2(16)O2, Ni(2)18O2 and Ni(2)16O18O isotopic data for five fundamental transitions enable a discussion of structural parameters for matrix-isolated Ni2O2 in its cyclic ground state. Analysis of the nickel isotopic effects on the 58,60Ni2(16)O18O fundamentals suggest an elongated rhombic structure with a Ni-O bond force constant (240+/-10 N m-1) and NiONi bond angles around 79 degrees. The latter points to a Ni-Ni internuclear distance shorter than the O-O one. Low-lying singlet, triplet and quintet states have been studied using density functional theory with an unrestricted wave function and broken symmetry formalism. The high spin states and closed shell singlet states have been also investigated at the CCSD(T) level. The Ni2O2 ground state is calculated to be an antiferromagnetic singlet state with all the hybrid functionals. The first order properties (energies, geometry) calculated with a hybrid functional are very similar when different exchange-correlation functionals with different exact exchange fractions are used and the calculated ground state geometry (NiONi bond angle near 80 degrees, NiO bond distance around 179.5 pm) is in good agreement with the experimental estimate. Nevertheless, a correct reproduction of the experimental vibrational properties is found only when a hybrid functional containing an exact exchange fraction in the 0.4-0.5 range is used. The orbital and topological bonding analyses of Ni2O2 reveal that the relatively short Ni-Ni internuclear distance within the molecule should not be interpreted as a remaining metal-metal bonding interaction, but clearly indicate that the bonding driving force is due to the formation of four strong and highly polarized Ni-O bonds. Even in such an early stage of metal oxidation, the Ni-Ni interaction has virtually disappeared. 相似文献
82.
Richelle M Darimont C Piguet-Welsch C Fay LB 《Rapid communications in mass spectrometry : RCM》2004,18(7):795-798
This paper presents a high-throughput method for the simultaneous determination of deuterium and oxygen-18 (18O) enrichment of water samples isolated from blood. This analytical method enables rapid and simple determination of these enrichments of microgram quantities of water. Water is converted into hydrogen and carbon monoxide gases by the use of a high-temperature conversion elemental analyzer (TC-EA), that are then transferred on-line into the isotope ratio mass spectrometer. Accuracy determined with the standard light Antartic precipitation (SLAP) and Greenland ice sheet precipitation (GISP) is reliable for deuterium and 18O enrichments. The range of linearity is from 0 up to 0.09 atom percent excess (APE, i.e. -78 up to 5725 delta per mil (dpm)) for deuterium enrichment and from 0 up to 0.17 APE (-11 up to 890 dpm) for 18O enrichment. Memory effects do exist but can be avoided by analyzing the biological samples in quintuplet. This method allows the determination of 1440 samples per week, i.e. 288 biological samples per week. 相似文献
83.
84.
We investigate nonlinear oscillations in a fourth-order partialdifferential equation which models a suspension bridge. Previouswork establishes multiple periodic solutions when a parameterexceeds a certain eigenvalue. In this paper, we use Leray-Schauderdegree theory to prove that if the parameter is increased further,beyond a second eigenvalue, then additional solutions are created. 相似文献
85.
A. Schweers F. Oldenburg Schern Gorli A. Grenz J. Pien G. Maurice D. Florentin L. C. Janse A. C. Fay Glenn A. Aikins und W. L. Davies 《Fresenius' Journal of Analytical Chemistry》1933,92(7-8):309-312
Ohne Zusammenfassung 相似文献
86.
In this study Plackett–Burman designs have been used to find the optimum conditions for separation of 15 phenolic compounds by LC. The responses used were the minimum resolution between two peaks and the analysis time. The adopted factors and experimental field were organic modifier (MeOH or ACN), percentage of acetic acid in the aqueous phase, flow rate, gradient with ten steps of percentage increase of the organic component of the mobile phase, and ten factors representing the duration of the steps. Use of Plackett–Burman designs achieved separation of the phenolic compounds within 45 min. 相似文献
87.
Fay JP Guaita MS Danelón JL Chifflet S Wawrzkiewicz M Fernández HM Ross DA 《Journal of AOAC International》2005,88(4):995-997
The objective of this work was to compare the traditional Van Soest's procedure to analyze neutral detergent fibers (NDF) and acid detergent fibers (ADF) using filtering crucibles (VS) with a semiautomatic method which uses filter bags in an ANKOM Technology Corp. instrument (ANK). Nine ruminant feeds widely used in the temperate region of Argentina were analyzed: soybean meal expeller, alfalfa, pasture silage, ryegrass, corn silage, weeping lovegrass, tall wheatgrass, guinea grass, and barley grass. Four runs were done for each technique and feed. The comparison of ADF and NDF means by the means test for paired samples showed no significant differences between techniques (alpha = 0.01). The variability among runs was greater with the VS method than the ANK, both for NDF, standard deviation (SD) = 0.71 vs 0.39, and for ADF, SD = 0.83 vs 0.56, but the differences were not significant. The linear regressions were VS = 1.43 + 0.95 ANK; R2 = 0.99, and VS = 0.53 + 0.98 ANK; R2 = 0.99 for NDF and ADF, respectively, which indicated a strong linear relationship among the results of both procedures. It was concluded that the ANK procedure gave results comparable to those of the VS method when ruminant feeds from the temperate region of Argentina were analyzed. 相似文献
88.
The use of semiconductors, as photoelectrodes in electrolytic cells for the electrolysis of water, is described and the results
reported in the literature for various semiconductors are reviewed. The most important properties of the semiconductor are
shown to be the band-gap energyE
g
, and the flat-band potentialU
fb
. The semiconductor absorbs photons that are more energetic than the band-gap energy and creates electronhole pairs. These
charge carriers can be separated before recombination by the electric field at the semiconductor-electrolyte interface. For
electrolysis to proceed, the potential corresponding to the band gap must appreciably exceed the standard potential for the
electrolysis of water, 1.23 volts. In addition, the flat-band potential must be more negative than the hydrogen potential
or an external bias voltage is required. The semiconductor must not corrode under the operating conditions and must permit
transfer of the minority carrier to the electrolyte. The current theories of charge transfer and reaction mechanism are discussed.
Many semiconductive oxides have been tested as photoanodes and found to be stable. However, only those compounds that have
band gaps of ca. 3 eV have been found to have flat-band potentials that are more negative than the hydrogen potential. These
compounds will electrolyse water, without additional bias voltage, but are inefficient absorbers of solar energy. Experiments
withp-type photocathodes,p andn combinations and various special configurations are also described. The paper concludes with a general discussion of the
practical prospects of photoelectrolysis in comparison with solid-state solar cells. 相似文献
89.
We calculate the effect of scattering on the static, exchange enhanced, spin susceptibility and show that, in particular, spin-orbit scattering leads to a reduction of the giant moments and spin glass freezing temperature due to dilute magnetic impurities. The harmful spin fluctuation contribution to the intragrain pairing interaction is strongly reduced opening the way for BCS superconductivity. We are thus able to explain the superconducting and magnetic properties recently observed in granular Pt as being due to scattering effects in single small grains. 相似文献
90.
This study describes a rapid and simple method to determine short-chain fatty acid (SCFA) concentrations and their isotopic enrichments (M(0) + 1 and M(0) + 2) in human plasma. Sample preparation involves SCFA extraction and derivatization with 1-(tert-butyldimethylsilyl)imidazole. Gas chromatography/mass spectrometry was performed using chemical ionization with ammonia as the reagent gas. Outstanding resolution, excellent linearity and good detection limits were obtained. Inter-assay and intra-assay repeatability was below 10% and 3% respectively for SCFA concentration. Inter-assay repeatability was below 5%, 4%, 6%, and 14% for isotopic enrichment determination of [1-(13)C]acetate and [1,2-(13)C(2)]acetate, [1-(13)C]propionate and [1-(13)C]butyrate respectively, with intra-assay being below 6%. Such SCFA concentrations and isotopic enrichments were determined in the plasma of rats infused with a (13)C-labeled SCFA. The turnovers of acetate, propionate and butyrate in rats were 19 micromol kg(-1) min(-1), 2.6 micromol kg(-1) min(-1), 0.3 micromol kg(-1) min(-1) respectively. 相似文献