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51.
The nonmetal-to-metal transition in dense fluid helium is discussed, which has been, in analogy to metallization of hydrogen, predicted as first-order plasma phase transition using chemical models for the equation of state and plasma composition. However, recent ab initio simulations performed for dense fluid helium indicate that this transition is continuous in the considered regime, without a density jump and latent heat as characteristic of a first-order phase transition. Implications for some astrophysical plasmas are discussed. 相似文献
52.
53.
《Journal of computational science》2014,5(4):568-575
Mechanisms for the decomposition reaction of ethylamine, CH3CH2NH2, were investigated using ab initio, DFT, and RRKM calculations. Optimized geometries of reactants, transition states, intermediates, and products were determined at HF, MP2, and B3LYP levels of theory using the 6-31G(d) and 6-31+G(d) basis sets. Single point energies were also determined at G3MP2B3 and G3B3 levels of theory. Thermodynamic properties, activation energies, enthalpies and Gibbs energies of activation were calculated for each reaction pathway investigated. Intrinsic reaction coordinate (IRC) analysis was performed to characterize the transition states on the potential energy surface. The conformational change and planarity of the ethylamine moiety along with the twist angle of the amino group about the CN axis are examined. Four pathways for the decomposition reaction of ethylamine were studied. All pathways involve a 1,2-elimination reaction and 1,3-proton shift to produce ethene, ethanimine, ethenamine, and methanimine. All pathways are single-step mechanisms. Elimination of the NH3 dominates the decomposition behavior up to 1200 K whereas after this temperature, secession of the C–N gradually holds more importance. While pathways signifying departures of NH3 and NH2 exhibit pressure-dependent behavior, branching ratios for these two channels are generally not influenced by variation in pressure higher than the atmospheric pressure. 相似文献
54.
The Italian health insurance market is currently undersized. The paucity of assured data and the discontinuous statistical surveys carried out by the National Institute of Statistics (ISTAT) represent one of the main obstacles to the insurance market development. The paper sets forth a parametric model to estimate technical basis for health insurance policies when data are limited and only aggregated information on mortality and morbidity is available. The probabilistic framework is based on a multiple state continuous and time inhomogeneous Markov model. We provide an estimate of transition intensities from the healthy state to the sickness state when only prevalence rates of sickness are available, according to an extension and modification of the methodology proposed in Olivieri (1996) for Long Term Care insurance. We assume that mortality intensity of both healthy and sick lives is modelled by two independent Gompertz–Makeham models. 相似文献
55.
Norberto Manfredi Alberto Bianchi Valerio Causin Riccardo Ruffo Roberto Simonutti Alessandro Abbotto 《Journal of polymer science. Part A, Polymer chemistry》2014,52(5):719-727
The first use of PSn‐b‐PEOm‐b‐PSn block copolymers (PS = polystyrene, PEO = poly(ethylene oxide)) as solid hosts for iodine/iodide electrolytes in dye‐sensitized solar cells (DSSCs) is described. Using the benchmark photosensitizer N719, DSSC based on the quasi solid‐state electrolytes afforded efficiencies up to 6.7%, to be compared with an efficiency of 7.3% obtained in similar conditions with a conventional iodine/iodide liquid electrolyte. By varying the PS:PEO relative volume ratio in the block copolymers different properties and morphologies were obtained. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2014 , 52, 719–727 相似文献
56.
Feng‐Yang Bai Xiao‐Le Zhu Zi‐Man Jia Xu Wang Yan‐Qiu Sun Prof. Rong‐Shun Wang Prof. Xiu‐Mei Pan 《Chemphyschem》2015,16(8):1768-1776
The mechanism and kinetics of the reactions of CF3COOCH2CH3, CF2HCOOCH3, and CF3COOCH3 with Cl and OH radicals are studied using the B3LYP, MP2, BHandHLYP, and M06‐2X methods with the 6‐311G(d,p) basis set. The study is further refined by using the CCSD(T) and QCISD(T)/6‐311++G(d,p) methods. Seven hydrogen‐abstraction channels are found. All the rate constants, computed by a dual‐level direct method with a small‐curvature tunneling correction, are in good agreement with the experimental data. The tunneling effect is found to be important for the calculated rate constants in the low‐temperature range. For the reaction of CF3COOCH2CH3+Cl, H‐abstraction from the CH2 group is found to be the dominant reaction channel. The standard enthalpies of formation for the species are also calculated. The Arrhenius expressions are fitted within 200–1000 K as kT(1)=8.4×10?20T 2.63exp(381.28/T), kT(2)=2.95×10?21T 3.13exp(?103.21/T), kT(3)=1.25×10?23T 3.37exp(791.98/T), and kT(4)=4.53×10?22T 3.07exp(465.00/T). 相似文献
57.
Prof. Dr. Suning Wang Deng‐Tao Yang Jiasheng Lu Hiroyuki Shimogawa Prof. Dr. Shaolong Gong Xiang Wang Soren K. Mellerup Prof. Dr. Atsushi Wakamiya Dr. Yi‐Lu Chang Prof. Dr. Chuluo Yang Prof. Dr. Zheng‐Hong Lu 《Angewandte Chemie (International ed. in English)》2015,54(50):15074-15078
New BN‐heterocyclic compounds have been found to undergo double arene photoelimination, forming rare yellow fluorescent BN‐pyrenes that contain two B? N units. Most significant is the discovery that the double arene elimination can also be driven by excitons generated electrically within electroluminescent (EL) devices, enabling the in situ solid‐state conversion of BN‐heterocycles to BN‐pyrenes and the use of BN‐pyrenes as emitters for EL devices. The in situ exciton‐driven elimination (EDE) phenomenon has also been observed for other BN‐heterocycles. 相似文献
58.
59.
Dr. Alessandra Alberti Dr. Ioannis Deretzis Dr. Giovanna Pellegrino Dr. Corrado Bongiorno Dr. Emanuele Smecca Dr. Giovanni Mannino Dr. Filippo Giannazzo Prof. Guglielmo Guido Condorelli Dr. Nobuya Sakai Prof. Tsutomu Miyasaka Dr. Corrado Spinella Dr. Antonino La Magna 《Chemphyschem》2015,16(14):3064-3071
We investigate the degradation path of MAPbI3 (MA=methylammonium) films over flat TiO2 substrates at room temperature by means of X‐ray diffraction, spectroscopic ellipsometry, X‐ray photoelectron spectroscopy, and high‐resolution transmission electron microscopy. The degradation dynamics is found to be similar in air and under vacuum conditions, which leads to the conclusion that the occurrence of intrinsic thermodynamic mechanisms is not necessarily linked to humidity. The process has an early stage, which drives the starting tetragonal lattice in the direction of a cubic atomic arrangement. This early stage is followed by a phase change towards PbI2. We describe how this degradation product is structurally coupled with the original MAPbI3 lattice through the orientation of its constituent PbI6 octahedra. Our results suggest a slight octahedral rearrangement after volatilization of HI+CH3NH2 or MAI, with a relatively low energy cost. Our experiments also clarify why reducing the interfaces and internal defects in the perovskite lattice enhances the stability of the material. 相似文献
60.
Anchoring Mechanism of ZnO Nanoparticles on Graphitic Carbon Nanofiber Surfaces through a Modified Co‐Precipitation Method to Improve Interfacial Contact and Photocatalytic Performance 下载免费PDF全文
Dr. Gowra Raghupathy Dillip Dr. Arghya Narayan Banerjee Dr. Veettikunnu Chandran Anitha Dr. Sang Woo Joo Dr. Bong Ki Min Dr. Sandesh Y. Sawant Dr. Moo Hwan Cho 《Chemphyschem》2015,16(15):3214-3232
A facile three‐step co‐precipitation method is developed to synthesize graphitic carbon nanofibers (CNFs) decorated with ZnO nanoparticles (NPs). By interchanging intermediate steps of the reaction processes, two kinds of nanohybrids are fabricated with stark morphological and physicochemical differences. The morphologies differ because of the different chemical environments of the NP/nanocluster formation. The hybrid with larger and non‐uniform ZnO nanocluster size is formed in liquid phase and resulted in considerable interfacial defects that deteriorate the charge‐transfer properties. The hybrid with smaller and uniform ZnO NPs was formed in a dry solid phase and produced near‐defect‐free interfaces, leading to efficient charge transfer for superior photocatalytic performance. The results broaden the understanding of the anchoring/bonding mechanism in ZnO/CNF hybrid formation and may facilitate further development of more effective exfoliation strategies for the preparation of high‐performance composites/hybrids. 相似文献