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111.
112.
Thin layers of (25–1000 Å) tin were evaporated onto a highly oriented polypropylene sheet. Two rates of deposition were used: 5 and 20 Å/s. For the more rapid deposition rate, a preferred orientation of tin was found in all cases. Here, the Sn a axis lay parallel to the polymer chain (polymer c axis). The same orientation relationship was found for the slower deposition rate, but only at lower Sn film thicknesses; at the higher film thicknesses, a random orientation of crystallites is found. Scanning electron micrographs show an equiaxed tin grain structure for the case of no preferred orientation and a platelet morphology for the case of preferred orientation, the thin dimension of the platelets lying perpendicular to the polymer chain axis. Although no clearcut evidence either for or against crystallographic epitaxy has been found, a plausible case for geometrical epitaxy is presented. 相似文献
113.
We examine a method for computing the change in free energy with temperature of a crystalline solid. In the method, the free-energy difference between nearby temperatures is calculated via overlap-sampling free-energy perturbation with Bennett's optimization. Coupled to this is a harmonically targeted perturbation that displaces the atoms in a manner consistent with the temperature change, such that for a harmonic system, the free-energy difference would be recovered with no error. A series of such perturbations can be assembled to bridge larger gaps in temperature. We test this harmonically targeted temperature perturbation (HTTP) method through the application to the inverse-power soft potential, u(r)=ε(σ/r)(n), over a range of temperatures up to the melting condition. Three exponent values (n=12, 9, and 6) for the potential are studied with different crystal structures, specifically face-centered cubic (fcc), body-centered cubic (bcc), and hexagonal close packing. Absolute free energies (classical only) for each system are obtained by implementing the series to near-zero temperature, where the harmonic model becomes very accurate. The HTTP method is shown to provide very precise results, with errors in the free energy smaller than two parts in 10(5). An analysis of the thermodynamic stability of the various structures in the infinite-system limit confirms previous findings. In particular, for n=12 and 9, the fcc structure is stable for all temperatures up to melting, and for n=6, the bcc crystal becomes stable relative to fcc for temperatures above kT/ε=0.802±0.001. The effects of vacancies and other defects are not considered in the analysis. 相似文献
114.
Leibfarth FA Schneider Y Lynd NA Schultz A Moon B Kramer EJ Bazan GC Hawker CJ 《Journal of the American Chemical Society》2010,132(42):14706-14709
The functionalization and cross-linking of polyethylene is synthetically challenging, commonly relying on highly optimized radical based postpolymerization strategies. To address these difficulties, a norbornene monomer containing Meldrum's acid is shown to be effectively copolymerized with polyethylene using a nickel α-iminocarbaxamidato complex, providing high-melting, semicrystalline polymers with a tunable incorporation of the functional comonomer. Upon heating the copolymer to common polyethylene processing temperatures, the thermolysis of Meldrum's acid to ketene provides the desired reactive group. This simple and versatile methodology does not require small molecule radical sources or catalysts, and the dimerization of the in situ generated ketenes is shown to provide tunable cross-linking densities in polyethylene. Subsequent rheological and tensile experiments illustrate the ability to tune cross-linked polyethylene properties by comonomer incorporation and elucidate valuable structure/property relationships in these materials. This study illustrates the power of well-defined and synthetically accessible functional groups in polyolefin synthesis and functionalization. 相似文献
115.
Clathculins A and B represent a new class of vic-diamine alkaloids containing a PA2 unit as the basic structure. We report the first total syntheses of 1 and 2, which confirm the assigned structure of each. Dependence of their NMR spectroscopic behavior as a function of protonation state has been observed. 相似文献
116.
Kauffmann-Weiss S Gruner ME Backen A Schultz L Entel P Fähler S 《Physical review letters》2011,107(20):206105
We exploit the intrinsic structural instability of the Fe(70)Pd(30) magnetic shape memory alloy to obtain functional epitaxial films exhibiting a self-organized nanostructure. We demonstrate that coherent epitaxial straining by 54% is possible. The combination of thin film experiments and large-scale first-principles calculations enables us to establish a lattice relaxation mechanism, which is not expected for stable materials. We identify a low twin boundary energy compared to a high elastic energy as key prerequisite for the adaptive nanotwinning. Our approach is versatile as it allows to control both, nanostructure and intrinsic properties for ferromagnetic, ferroelastic, and ferroelectric materials. 相似文献
117.
Björn Bieniek Darius Pohl Ludwig Schultz Bernd Rellinghaus 《Journal of nanoparticle research》2011,13(11):5935-5946
The near-surface oxidation-induced lattice relaxation and compositional changes of FeNi alloy nano-particles are investigated.
Using a newly developed transfer system, the particle structure was characterised by means of aberration-corrected HR-TEM
prior to exposing the particles to ambient air. This allows for a comparison of oxidised and un-oxidised particles, respectively.
Independent of the oxidation, the surface-near and/or interface-near metal lattice was found to be expanded by up to 3%. EELS
profiles clearly reveal an enrichment of Fe at the particle surfaces. MD simulations in combination with HR-TEM contrast simulations
were conducted to investigate the effect of the Fe enrichment on the structural relaxation. The results show that a surface-near
over-stoichiometric enrichment of Fe indeed causes a dilation that counteracts a compression of the lattice at the particle
surface as obtained for homogeneously alloyed particles. Besides, the large lattice mismatch between the metallic cores and
the NiFe2O4 shells causes the formation of step dislocations in the close vicinities of the interface. In essence, the surface-near lattice
relaxation in oxide free particles is found to be due to a segregation of Fe to the surface, whereas in the case of shell–core
particles, no systematic influence of the oxide on the lattice relaxation was found. 相似文献
118.
E. Arushanov S. Levcenko G. Fuchs B. Holzapfel S.-L. Drechsler L. Schultz 《Physica C: Superconductivity and its Applications》2011,471(7-8):237-241
We show that the zero-field normal-state resistivity of temperature-dependent resistivity ρ(T) of SrFe2?xNixAs2 can be reproduced by the expression ρ(T) = ρ0 + c T exp(?2Δ/T). ρ(T) can be scaled using both this expression where the energy scale Δ, c and the residual resistivity ρ0 are scaling parameters and a recently proposed model-independent scaling method (H.G. Luo, Y.H. Su, T. Xiang, Phys. Rev. B 77 (2008) 014529). The scaling parameters have been calculated and the compositional variation of 2Δ(x) has been determined. This dependence show almost a linear decreasing in the underdoped regime similar to that reported for cuprates. The existence of a universal metallic ρ(T) curve in a wide temperature range which, however, is restricted for the underdoped compounds to temperatures above a structural and anitiferromagnetic transition is interpreted as an indication of a single mechanism which dominates the scattering of the charge carriers in SrFe2?xNixAs2 (x = 0–0.3). 相似文献
119.
W E Steiner B H Clowers K Fuhrer M Gonin L M Matz W F Siems A J Schultz H H Hill 《Rapid communications in mass spectrometry : RCM》2001,15(23):2221-2226
Rapid screening and identification of drug and other mixtures are possible using a novel ambient pressure high-resolution ion mobility (APIMS) orthogonal reflector time-of-flight mass spectrometer (TOFMS). Departing ions from the APIMS drift tube traversed a pressure interface between the APIMS and TOFMS where they were subjected to numerous gas collisions that could produce selective fragmentation. By increasing the accelerating field in the pressure interface region, the ions generated using water-cooled electrospray ionization (ESI) underwent collision-induced dissociation (CID). Mixtures of ESI ions were separated by APIMS based on their respective size-to-charge (s/z) ratios while CID and analysis of mass-to-charge (m/z) ratios occurred in the pressure interface and TOFMS. Product ions that were formed in this pressure interface region could be readily assigned to precursor ions by matching the mobility drift times. This process was demonstrated by the examination of a mixture of amphetamines and the resulting fragmentation patterns of the mobility-separated precursor ion species [M + H](+). 相似文献
120.