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991.
Subramanian S Devasahayam N McMillan A Matsumoto S Munasinghe JP Saito K Mitchell JB Chandramouli GV Krishna MC 《Journal of magnetic resonance (San Diego, Calif. : 1997)》2012,214(1):244-251
Oxygen maps derived from electron paramagnetic resonance spectral-spatial imaging (EPRI) are based upon the relaxivity of molecular oxygen with paramagnetic spin probes. This technique can be combined with MRI to facilitate mapping of pO(2) values in specific anatomic locations with high precision. The co-registration procedure, which matches the physical and digital dimensions of EPR and MR images, may present the pO(2) map at the higher MRI resolution, exaggerating the spatial resolution of oxygen, making it difficult to precisely distinguish hypoxic regions from normoxic regions. The latter distinction is critical in monitoring the treatment of cancer by radiation and chemotherapy, since it is well-established that hypoxic regions are three or four times more resistant to treatment compared to normoxic regions. The aim of this article is to describe pO(2) maps based on the intrinsic resolution of EPRI. A spectral parameter that affects the intrinsic spatial resolution of EPRI is the full width at half maximum (FWHM) height of the gradient-free EPR absorption line in frequency-encoded imaging. In single point imaging too, the transverse relaxation times (T(2)(?)) limit the resolution since the signal decays by exp(-t(p)/T(2)(?)) where the delay time after excitation pulse, t(p), is related to the resolution. Although the spin densities of two point objects may be resolved at this separation, it is inadequate to evaluate quantitative changes of pO(2) levels since the linewidths are proportionately affected by pO(2). A spatial separation of at least twice this resolution is necessary to correctly identify a change in pO(2) level. In addition, the pO(2) values are blurred by uncertainties arising from spectral dimensions. Blurring due to noise and low resolution modulates the pO(2) levels at the boundaries of hypoxic and normoxic regions resulting in higher apparent pO(2) levels in hypoxic regions. Therefore, specification of intrinsic resolution and pO(2) uncertainties are necessary to interpret digitally processed pO(2) illustrations. 相似文献
992.
Jacob Powell Domenic Valenti Harley Bobnar Erika Drain Blaine Elliott Sydney Frank Tyler McCullough Sean Moore Andrew Kettring Robbie Iuliucci James K. Harper 《Magnetic resonance in chemistry : MRC》2017,55(11):979-989
This study explores the feasibility of using a combination of experimental and theoretical 1‐bond 13C─13C scalar couplings (1JCC) to establish structure in organic compounds, including unknowns. Historically, nJCC and nJCH studies have emphasized 2 and 3‐bond couplings, yet 1JCC couplings exhibit significantly larger variations. Moreover, recent improvements in experimental measurement and data processing methods have made 1JCC data more available. Herein, an approach is evaluated in which a collection of theoretical structures is created from a partial nuclear magnetic resonance structural characterization. Computed 1JCC values are compared to experimental data to identify candidates giving the best agreement. This process requires knowledge of the error in theoretical methods, thus the B3LYP, B3PW91, and PBE0 functionals are evaluated by comparing to 27 experimental values from INADEQUATE. Respective errors of ±1.2, ±3.8, and ±2.3 Hz are observed. An initial test of this methodology involves the natural product 5‐methylmellein. In this case, only a single candidate matches experimental data with high statistical confidence. This analysis establishes the intramolecular hydrogen‐bonding arrangement, ring heteroatom identity, and conformation at one position. This approach is then extended to hydroheptelidic acid, a natural product not fully characterized in prior studies. The experimental/theoretical approach proposed herein identifies a single best‐fit structure from among 26 candidates and establishes, for the first time, 1 configuration and 3 conformations to complete the characterization. These results suggest that accurate and complete structural characterizations of many moderately sized organic structures (<800 Da) may be possible using only 1JCC data. 相似文献
993.
Nimmy R. Mammoottil James F. Reuther Dumindika A. Siriwardane Oleg V. Kulikov Bruce M. Novak 《Journal of polymer science. Part A, Polymer chemistry》2017,55(18):2915-2934
Described herein is a comprehensive survey on the most recent advancements in polycarbodiimide synthetic methodologies, structure determination, property design, and self-assembly. In particular, the 15N-isotopic enrichment of polycarbodiimides is detailed along with the use of 15N NMR to identify the regioregularity and mechanism of chiroptical switching in polycarbodiimides. Furthermore, the new Ni(II) mediated “living” polymerization is explained along with its utilization in the incorporation of polycarbodiimides into block copolymers, graft copolymers, and star polymers. Finally, we review the recent discoveries focusing on the highly tunable self-assembly behaviors of polycarbodiimide homopolymers and copolymers. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2017 , 55, 2915–2934 相似文献
994.
A new photoelastic model for studying fatigue crack closure 总被引:1,自引:0,他引:1
The photoelastic analysis of crack tip stress intensity factors has been historically developed for use on sharp notches in
brittle materials that idealize the cracked structure. This approach, while useful, is not applicable to cases where residual
effects of fatigue crack development (e.g., plasticity, surface roughness) affect the applied stress intensity range. A photoelastic
model of these fatigue processes has been developed using polycarbonate, which is sufficiently ductile to allow the growth
of a fatigue crack. The resultant stress field has been modeled mathematically using the stress potential function approach
of Muskhelishvili to predict the stresses near a loaded but closed crack in an elastic body. The model was fitted to full-field
photoelastic data using a combination of a generic algorithm and the downhill simplex method. The technique offers a significant
advance in the ability to characterize the behavior of fatigue cracks with plasticity-induced closure, and hence to gain new
insights into the associated mechanisms. 相似文献
995.
This paper describes a combined experimental and numerical study of scalar transport in spatially developing, two-stream,
turbulent mixing layers with velocity ratios of approximately 2:1. The experimental mixing layer was created by an S-shaped
splitter plate mounted in a wind tunnel, and the concentration field was realized by releasing incense smoke into the high-speed
side boundary layer above the splitter plate. Simultaneous measurements of the velocity and concentration fields were performed.
A 12-sensor hot-wire probe was used to measure the velocity field and its gradients, while the concentration field was recorded
with digital photographs of the laser-illuminated smoke. In parallel, a large-eddy simulation (LES) of the spatially developing
mixing layer was carried out. Auxiliary turbulent boundary layer LES were used to provide high quality inflow boundary conditions
for the velocity and concentration fields. By synchronizing the velocity and concentration measurements, concentration fluxes
were also determined. Octant analysis based on the sign combinations of the velocity and concentration fuctuations was performed
on the flux data to investigate the scalar transport processes. It was found that octants compatible with mean gradient transport
of the scalar contribute most to the scalar fluxes. Conditional planar averages of scalar and momentum fluxes were obtained
to determine their spatial distribution with respect to the organized roller and rib vortices of the mixing layer, and distinct
patterns were observed. The simulation provided additional insight about the flow and scalar flux distribution topology. This
topology was found to be partially compatible with simple models of roller and rib vortices that transport the scalar in a
mean gradient sense. 相似文献
996.
The transport of monodisperse as well as polydisperse colloid suspensions in a two-dimensional, water saturated fracture with spatially variable and anisotropic aperture is investigated with a particle tracking model. Both neutrally buoyant and dense colloid suspensions are considered. Although flow and transport in fractured subsurface formations have been studied extensively by numerous investigators, the transport of dense, polydisperse colloid suspensions in a fracture with spatially variable and anisotropic aperture has not been previously explored. Simulated snapshots and breakthrough curves of ensemble averages of several realizations of a log-normally distributed aperture field show that polydisperse colloids exhibit greater spreading than monodisperse colloids, and dense colloids show greater retardation than neutrally buoyant colloids. Moreover, it is demonstrated that aperture anisotropy oriented along the flow direction substantially increases colloid spreading; whereas, aperture anisotropy oriented transverse to the flow direction retards colloid movement. 相似文献
997.
The boundary-layer equations for axisymmetric stagnation point flow of a power-law fluid are solved by a similarity transformation, and values of the wall shear rate are obtained. Theoretical expressions for local and average Sherwood numbers are derived from the convective diffusion equation for systems with high Schmidt numbers. The results can be used to predict diffusion coefficients of dilute species in fluids with specified power-law characteristics. 相似文献
998.
Dr. Sunewang R. Wang Dr. Merle Arrowsmith Julian Böhnke Prof. Dr. Holger Braunschweig Dr. Theresa Dellermann Dr. Rian D. Dewhurst Hauke Kelch Dr. Ivo Krummenacher James D. Mattock Jonas H. Müssig Torsten Thiess Dr. Alfredo Vargas Dr. Jiji Zhang 《Angewandte Chemie (International ed. in English)》2017,56(27):8009-8013
The diborene 1 was synthesized by reduction of a mixture of 1,2-di-9-anthryl-1,2-dibromodiborane(4) ( 6 ) and trimethylphosphine with potassium graphite. The X-ray structure of 1 shows the two anthryl rings to be parallel and their π(C14) systems perpendicular to the diborene π(B=B) system. This twisted conformation allows for intercalation of the relatively high-lying π(B=B) orbital and the low-lying π* orbital of the anthryl moiety with no significant conjugation, resulting in a small HOMO–LUMO gap (HLG) and ultimately a C−H borylation of the anthryl unit. The HLG of 1 was estimated to be 1.57 eV from the onset of the long wavelength band in its UV/Vis absorption spectrum (THF, λonset=788 nm). The oxidation of 1 with elemental selenium afforded diboraselenirane 8 in quantitative yield. By oxidative abstraction of one phosphine ligand by another equivalent of elemental selenium, the B−B and C1−H bonds of 8 were cleaved to give the cyclic 1,9-diborylanthracene 9 . 相似文献
999.
Marco Baity-Jesi Carl P. Goodrich Andrea J. Liu Sidney R. Nagel James P. Sethna 《Journal of statistical physics》2017,167(3-4):735-748
We study the shear jamming of athermal frictionless soft spheres, and find that in the thermodynamic limit, a shear-jammed state exists with different elastic properties from the isotropically-jammed state. For example, shear-jammed states can have a non-zero residual shear stress in the thermodynamic limit that arises from long-range stress-stress correlations. As a result, the ratio of the shear and bulk moduli, which in isotropically-jammed systems vanishes as the jamming transition is approached from above, instead approaches a constant. Despite these striking differences, we argue that in a deeper sense, the shear jamming and isotropic jamming transitions actually have the same symmetry, and that the differences can be fully understood by rotating the six-dimensional basis of the elastic modulus tensor. 相似文献