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991.
Silver-containing layered networks of the form [Ag(L)] (L = 4-pyridinesulfonate or p-toluenesulfonate) were treated with primary amines in different ratios. The structures of the parent supramolecular networks are well-known; however, their interactions with primary amines lead to the formation of new layered materials for which single-crystal X-ray structures cannot be obtained. Solid-state (109)Ag, (15)N, and (13)C cross-polarization magic-angle spinning (CP/MAS) NMR experiments, in combination with powder X-ray diffraction experiments and ab initio calculations, are utilized to investigate the interactions between the primary amines and the parent materials, and to propose structural models for the new materials. (109)Ag chemical shift (CS) tensor parameters are extremely sensitive to changes in silver environments; hence, (1)H-(109)Ag CP/MAS NMR experiments are used to distinguish and characterize silver sites. The combination of (109)Ag and (15)N NMR experiments on starting materials and samples prepared with both (15)N-labeled and unlabeled amines permits the accurate measurements of indirect (1)J((109)Ag,(15)N) and (1)J((109)Ag,(14)N) spin-spin coupling constants, providing further information on structure and bonding in these systems. First principles calculations of silver CS tensors and (1)J((109)Ag,(14)N) coupling constants in model complexes aid in formulating the proposed structural models for the new materials, which are largely comprised of layers of silver-diamine cations. 相似文献
992.
Didit Yudistira Andreas Boes Benjamin Dumas Amgad R. Rezk Morteza Yousefi Bahram Djafari‐Rouhani Leslie Y. Yeo Arnan Mitchell 《Annalen der Physik》2016,528(5):365-372
Surface phonon cavities that are homogenous in both mechanical and dielectric properties are reported. The cavities are formed by the placement of a defect of a single domain within periodic domain inversion of single crystal piezoelectric lithium niobate that exhibits surface phononic bandgap through the phonon‐polariton coupling. Surface cavity resonances are observed within the bandgap, which manifest in entrapment of phonon‐polariton within the defect. In addition to demonstrating that the observed resonances are non‐radiative and decoupled to bulk radiation, which is critical for high Q cavities, it is also shown the possibility to tune the surface cavity resonance spectra simply by varying the defect width. Such an ability to excite surface cavity resonance that is non‐radiative with simultaneous localization of the electric field together with the advantage of a cavity that is physically formed from a completely monolithic and uniform material offers unique opportunities for widespread applications for example in actuation, detection, and phonon lasing that can be fully integrated with other physical systems such as quantum acoustics, photonics, and microfluidics.
993.
Josep Díaz Leslie Ann Goldberg David Richerby Maria Serna 《Random Structures and Algorithms》2016,49(1):137-159
The Moran process models the spread of mutations in populations on graphs. We investigate the absorption time of the process, which is the time taken for a mutation introduced at a randomly chosen vertex to either spread to the whole population, or to become extinct. It is known that the expected absorption time for an advantageous mutation is on an n‐vertex undirected graph, which allows the behaviour of the process on undirected graphs to be analysed using the Markov chain Monte Carlo method. We show that this does not extend to directed graphs by exhibiting an infinite family of directed graphs for which the expected absorption time is exponential in the number of vertices. However, for regular directed graphs, we show that the expected absorption time is and . We exhibit families of graphs matching these bounds and give improved bounds for other families of graphs, based on isoperimetric number. Our results are obtained via stochastic dominations which we demonstrate by establishing a coupling in a related continuous‐time model. The coupling also implies several natural domination results regarding the fixation probability of the original (discrete‐time) process, resolving a conjecture of Shakarian, Roos and Johnson. © 2016 Wiley Periodicals, Inc. Random Struct. Alg., 49, 137–159, 2016 相似文献
994.
Leslie R. Pendrill 《Accreditation and quality assurance》2008,13(11):619-631
A discussion in economic terms of common rules in conformity assessment based on measurement is given. The present work extends
tools of sampling when using inspection by variable and attribute, such as the setting of acceptance quality limits (AQL)
and limiting quality limits (LQL), by including an economic decision theory approach, leading, amongst other things, to a
new ‘cost’ curve as a complement to the traditional operating characteristic curves of statistical significance testing. The
methodology is of general applicability but is illustrated in the present work in the simple case of homogeneously pre-packaged
goods priced linearly with the amount of content. The relation to the optimised uncertainty methodology is explained. Optimum
strategies for the supplier are illustrated in terms of minimising production and testing costs, while at the same time maintaining
satisfactory levels of customer satisfaction.
相似文献
Leslie R. PendrillEmail: |
995.
Field LD Li HL Dalgarno SJ Turner P 《Chemical communications (Cambridge, England)》2008,(14):1680-1682
The side-on bound metal complex of diazene cis-[Fe(NH[double bond]NH)(dmpe)(2)] was synthesised by reaction of [Fe(dmpe)(2)Cl(2)] with hydrazine in the presence of potassium graphite and characterised by (15)N NMR spectroscopy and X-ray crystallography. 相似文献
996.
The synthesis of nucleoside analogues incorporating 4-(5-pyrimidinyl)-1,2,3-triazole aglycons as expanded purine nucleobase mimics were accessed using the copper-catalyzed azide-alkyne Huisgen cycloaddition between a ribosyl azide and 5-alkynylpyrimidines. Depending on the nature of the alkyne employed, other nucleoside analogues that possess fluorescence or potential metal-binding properties were prepared. Computational studies were undertaken on the purine analogues and indicate that the heterocycles of the unfused nucleobase prefer a coplanar arrangement and the anti-glycosidic conformer is favoured in most instances. 相似文献
997.
Villalobos L Cao Z Fanwick PE Ren T 《Dalton transactions (Cambridge, England : 2003)》2012,41(2):644-650
Two new diruthenium(II,III) tetramidate compounds, Ru(2)(NHOCC(CH(3))(2))(4)Cl (1) and Ru(2)(NHOCCH(2)CH(3))(4)Cl (2) have been prepared and structurally characterized by X-ray crystallography. The activity of promoting sulfide oxygenation using simple oxidants such as hydrogen peroxide (H(2)O(2)) and tert-butyl hydroperoxide (TBHP) was studied. A UV-kinetics study indicated that the initial rates of 1 and 2 are comparable to the previously studied diruthenium tetracarboxylates in promoting TBHP oxygenation of methyl phenyl sulfide (MPS). Using excess oxidant and CH(3)CN as the solvent, organic sulfides MPS and diphenyl sulfide (PPS) were oxidized using 1 mol% of the catalytic species. Compound 1 is more effective than 2 in converting sulfides to sulfoxide under the same conditions. Fast conversion was achieved when the reactions were carried out in the solvent-free conditions, and the major oxidation product was the sulfoxide. The electronic structure of the title compounds was studied with DFT calculations to gain an understanding of the activation of peroxy reagents. 相似文献
998.
Queen WL Bloch ED Brown CM Hudson MR Mason JA Murray LJ Ramirez-Cuesta AJ Peterson VK Long JR 《Dalton transactions (Cambridge, England : 2003)》2012,41(14):4180-4187
The hydrogen storage properties of Fe(2)(dobdc) (dobdc(4-) = 2,5-dioxido-1,4-benzenedicarboxylate) and an oxidized analog, Fe(2)(O(2))(dobdc), have been examined using several complementary techniques, including low-pressure gas adsorption, neutron powder diffraction, and inelastic neutron scattering. These two metal-organic frameworks, which possess one-dimensional hexagonal channels decorated with unsaturated iron coordination sites, exhibit high initial isosteric heats of adsorption of -9.7(1) and -10.0(1) kJ mol(-1), respectively. Neutron powder diffraction has allowed the identification of three D(2) binding sites within the two frameworks, with the closest contacts corresponding to Fe-D(2) separations of 2.47(3) and 2.53(5) ?, respectively. Inelastic neutron scattering spectra, obtained from p-H(2) (para-H(2)) and D(2)-p-H(2) mixtures adsorbed in Fe(2)(dobdc), reveal weak interactions between two neighboring adsorption sites, a finding that is in opposition to a previous report of possible 'pairing' between neighboring H(2) molecules. 相似文献
999.
An LC/MS/MS-based multiresidue quantitative method was developed for the macrolides erythromycin A, neospiramycin I, oleandomycin, spiramycin I, tilmicosin, and tylosin A in porcine kidney tissues. The Canadian Food Inspection Agency (CFIA) had as part of its analytical scope an LC/UV method for quantification of residues of two macrolide antibiotics, tilmicosin and tylosin A, in the kidney, liver, and muscle of cattle, swine, and poultry. The method could not reliably detect concentrations below 10 microg/kg. To increase the scope of the CFIA's analytical capabilities, a sensitive multiresidue quantitative method for macrolide residues in food animal tissues was required. Porcine kidney samples were extracted with acetonitrile and alkaline buffer and cleaned-up using silica-based C18 SPE cartridges. Sample extracts were analyzed using LC/MS/MS with positive electrospray ionization. Fitness for purpose was verified in a single-laboratory validation study using a second analyst. The working analytical range was 5 to 50 microg/kg. LOD and LOQ were 0.5 to 0.6 microg/kg and 1.5 to 3.0 microg/kg, respectively. Limits of identification were 0.5 to 2.0 microg/kg. Relative intermediate precisions were 8 to 17%. Average absolute recoveries were 68 to 76%. 相似文献
1000.
Qian J Wani R Klomsiri C Poole LB Tsang AW Furdui CM 《Chemical communications (Cambridge, England)》2012,48(34):4091-4093
β-ketoesters are robust probes for labeling sulfenic acid (-SOH) proteins allowing quantitative cleavage of the tag for improved analysis of the labeled peptides by MS. 相似文献