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Dr. Jacorien Coetzee Dr. Deborah L. Dodds Prof. Jürgen Klankermayer Sandra Brosinski Prof. Walter Leitner Prof. Alexandra M. Z. Slawin Prof. David J. Cole‐Hamilton 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(33):11039-11050
Hydrogenation of amides in the presence of [Ru(acac)3] (acacH=2,4‐pentanedione), triphos [1,1,1‐tris‐ (diphenylphosphinomethyl)ethane] and methanesulfonic acid (MSA) produces secondary and tertiary amines with selectivities as high as 93 % provided that there is at least one aromatic ring on N. The system is also active for the synthesis of primary amines. In an attempt to probe the role of MSA and the mechanism of the reaction, a range of methanesulfonato complexes has been prepared from [Ru(acac)3], triphos and MSA, or from reactions of [RuX(OAc)(triphos)] (X=H or OAc) or [RuH2(CO)(triphos)] with MSA. Crystallographically characterised complexes include: [Ru(OAc‐κ1O)2(H2O)(triphos)], [Ru(OAc‐κ2O,O′)(CH3SO3‐κ1O)(triphos)], [Ru(CH3SO3‐κ1O)2(H2O)(triphos)] and [Ru2(μ‐CH3SO3)3(triphos)2][CH3SO3], whereas other complexes, such as [Ru(OAc‐κ1O)(OAc‐κ2O,O′)(triphos)], [Ru(CH3SO3‐κ1O)(CH3SO3‐κ2O,O′)(triphos)], H[Ru(CH3SO3‐κ1O)3(triphos)], [RuH(CH3SO3‐κ1O)(CO)(triphos)] and [RuH(CH3SO3‐κ2O,O′)(triphos)] have been characterised spectroscopically. The interactions between these various complexes and their relevance to the catalytic reactions are discussed. 相似文献
54.
Jiang X Arrington J Benmokhtar F Camsonne A Chen JP Choi S Chudakov E Cusanno F Deur A Dutta D Garibaldi F Gaskell D Gayou O Gilman R Glashauser C Hamilton D Hansen O Higinbotham DW Holt RJ de Jager CW Jones MK Kaufman LJ Kinney ER Kramer K Lagamba L de Leo R Lerose J Lhuillier D Lindgren R Liyanage N McCormick K Meziani ZE Michaels R Moffit B Monaghan P Nanda S Paschke KD Perdrisat CF Punjabi V Qattan IA Ransome RD Reimer PE Reitz B Saha A Schulte EC Sheyor R Slifer K Solvignon P Sulkosky V 《Physical review letters》2007,98(18):182302
We measured the angular dependence of the three recoil-proton polarization components in two-body photodisintegration of the deuteron at a photon energy of 2 GeV. These new data provide a benchmark for calculations based on quantum chromodynamics. Two of the five existing models have made predictions of polarization observables. Both explain the longitudinal polarization transfer satisfactorily. Transverse polarizations are not well described, but suggest isovector dominance. 相似文献
55.
A novel water-soluble solvatochromic molecule, 7-(dimethylamino)-2-fluorenesulfonate (2,7-DAFS), was prepared by a three-step
reaction from 2-nitrofluorene in good overall yield. The pH and solvent effects on the UV-VIS absorption and fluorescence
spectra of 2,7-DAFS have been studied. Protonation of the dimethylamino group switches the absorption from intramolecular
charge-transfer (ICT) to π → π* transition. The ground state pKa value of 2,7-DAFS was determined as 4.51. The fluorescence spectrum of the excited basic form, *(DAFS), shows a structureless
single band with a large Stokes shift, whereas that of the acidic form, *(+HDAFS), exhibits a structured band with a small Stokes shift. The emission intensities of the basic and acidic forms versus
pH/Ho plots show stretched sigmoidal curves and indicate that (1) the rate of deprotonation of *(+HDAFS) is comparable to the fluorescence decay of the species, and (2) the efficient proton-induced quenching of *(DAFS) fluorescence
occurs. The pKa* was estimated as −1.7 from the fluorescence titration curve. The fluorescence maximum of *(DAFS) is blue-shifted as the
polarity of solvent decreases. However, no clear dependency of the emission intensity and spectral half width, and thus fluorescence
quantum yield, on the solvent polarity was revealed. It appears that the fluorescence sensitivity of 2,7-DAFS is 15 ∼ 25 times
greater than the sensitivity of a widely utilized fluorescent probe, 5-(dimethylamino)-1-naphthalenesulfonate. This higher
sensitivity, together with the ease of derivatization, would provide the fluorene-based fluorescent molecules significant
advantages for a variety of applications. 相似文献
56.
Perini Nickson Delmonde Marcelo V. F. Ranjan Chinmoy Varela Hamilton 《Journal of Solid State Electrochemistry》2020,24(8):1811-1818
Journal of Solid State Electrochemistry - The characteristics of the electrochemical oscillations that emerge along the catalytic oxidation of small organic molecules critically depend on the... 相似文献
57.
J. Galy D. J. Hamilton C. Normand 《The European physical journal. Special topics》2009,175(1):147-152
In the last decade or so, an evolution in experimental relativistic laser-plasma physics has led to highly sophisticated lasers
which are now capable of generating ultra-short pulses and can be focused to intensities in excess of 1021 W cm-2. The laser interaction with solid or gas targets can generate collimated beams of highly energetic electrons, protons and
ions. These high-intensity laser systems, therefore, turn out to be versatile and powerful sources of radiation and high-energy
particles, without recourse to large-scale facilities such as nuclear reactors or particle accelerators. The potential to
induce various kinds of nuclear reactions with laser-induced radiation fields has been demonstrated at several laboratories
in recent years. The present paper lays out a comprehensive overview of nuclear reactions induced by high-intensity laser
matter interactions. Mechanisms for electron, proton and ion acceleration, in addition to secondary bremsstrahlung, positron
and neutron production, are addressed, with a focus on the types of nuclear reactions that are possible and potential applications.
Discussion of the extrapolation of these processes and applications to the next generation of table-top lasers under construction
is also presented. 相似文献
58.
J. H. Northern A. W. J. Thompson M. L. Hamilton P. Ewart 《Applied physics. B, Lasers and optics》2013,111(4):627-635
The detection of multiple species using a single laser and single detector employing multi-mode absorption spectroscopy (MUMAS) is reported. An in-house constructed, diode-pumped, Er:Yb:glass micro-laser operating at 1,565 nm with 10 modes separated by 18 GHz was used to record MUMAS signals in a gas mixture containing C2H2, N2O and CO. The components of the mixture were detected simultaneously by identifying multiple transitions in each of the species. By using temperature- and pressure-dependent modelled spectral fits to the data, partial pressures of each species in the mixture were determined with an uncertainty of ±2 %. 相似文献
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[reaction: see text] Data are presented indicating that the potent antitumor activity of 2-crotonyloxymethyl-(4R,5R,6R)-4,5,6-trihydroxy-2-cyclohexenone (COTC) and 2-crotonyloxymethyl-2-cyclohexenone (COMC) is not likely the result of glyoxalase I inhibition, as has long been assumed. An alternative hypothesis is presented, based on the finding that COMC is a substrate for human glutathionyl transferase, which produces a transient, highly electrophilic glutathionylated 2-exomethylenecyclohexanone that can covalently modify proteins and nucleic acids. 相似文献