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631.
Bledowski M Wang L Ramakrishnan A Khavryuchenko OV Khavryuchenko VD Ricci PC Strunk J Cremer T Kolbeck C Beranek R 《Physical chemistry chemical physics : PCCP》2011,13(48):21511-21519
We investigated photoelectrodes based on TiO(2)-polyheptazine hybrid materials. Since both TiO(2) and polyheptazine are extremely chemically stable, these materials are highly promising candidates for fabrication of photoanodes for water photooxidation. The properties of the hybrids were experimentally determined by a careful analysis of optical absorption spectra, luminescence properties and photoelectrochemical measurements, and corroborated by quantum chemical calculations. We provide for the first time clear experimental evidence for the formation of an interfacial charge-transfer complex between polyheptazine (donor) and TiO(2) (acceptor), which is responsible for a significant red shift of absorption and photocurrent response of the hybrid as compared to both of the single components. The direct optical charge transfer from the HOMO of polyheptazine to the conduction band edge of TiO(2) gives rise to an absorption band centered at 2.3 eV (540 nm). The estimated potential of photogenerated holes (+1.7 V vs. NHE, pH 7) allows for photooxidation of water (+0.82 V vs. NHE, pH 7) as evidenced by visible light-driven (λ > 420 nm) evolution of dioxygen on hybrid electrodes modified with IrO(2) nanoparticles as a co-catalyst. The quantum-chemical simulations demonstrate that the TiO(2)-polyheptazine interface is a complex and flexible system energetically favorable for proton-transfer processes required for water oxidation. Apart from water splitting, this type of hybrid materials may also find further applications in a broader research area of solar energy conversion and photo-responsive devices. 相似文献
632.
Laurent Desvillettes François Golse Valeria Ricci 《Journal of statistical physics》2008,131(5):941-967
We propose a mathematical derivation of Brinkman’s force for a cloud of particles immersed in an incompressible viscous fluid.
Specifically, we consider the Stokes or steady Navier-Stokes equations in a bounded domain Ω⊂ℝ3 for the velocity field u of an incompressible fluid with kinematic viscosity ν and density 1. Brinkman’s force consists of a source term 6π
ν
j where j is the current density of the particles, and of a friction term 6π
ν
ρ
u where ρ is the number density of particles. These additional terms in the motion equation for the fluid are obtained from the Stokes
or steady Navier-Stokes equations set in Ω minus the disjoint union of N balls of radius ε=1/N in the large N limit with no-slip boundary condition. The number density ρ and current density j are obtained from the limiting phase space empirical measure
, where x
k
is the center of the k-th ball and v
k
its instantaneous velocity. This can be seen as a generalization of Allaire’s result in [Arch. Ration. Mech. Anal. 113:209–259,
[1991]] who considered the case of periodically distributed x
k
s with v
k
=0, and our proof is based on slightly simpler though similar homogenization arguments. Similar equations are used for describing
the fluid phase in various models for sprays. 相似文献
633.
634.
In the last decade permutation entropy (PE) has become a popular tool to analyze the degree of randomness within a time series. In typical applications, changes in the dynamics of a source are inferred by observing changes of PE computed on different time series generated by that source. However, most works neglect the crucial question related to the statistical significance of these changes. The main reason probably lies in the difficulty of assessing, out of a single time series, not only the PE value, but also its uncertainty. In this paper we propose a method to overcome this issue by using generation of surrogate time series. The analysis conducted on both synthetic and experimental time series shows the reliability of the approach, which can be promptly implemented by means of widely available numerical tools. The method is computationally affordable for a broad range of users. 相似文献
635.
Maria Carta Leonarda Vugrin Dr. Goran Miletić Dr. Marina Juribašić Kulcsár Prof. Dr. Pier Carlo Ricci Dr. Ivan Halasz Prof. Dr. Francesco Delogu 《Angewandte Chemie (International ed. in English)》2023,62(33):e202308046
Typically induced by the mechanical processing of powders in ball mills, mechanochemical transformations are considered to result from the application of mechanical force to solid reactants. However, the undeniable deep connection between the dynamic compaction of powders during impacts and the overall transformation degree has yet to be disclosed. In the present work, we show that the square planar bis(dibenzoylmethanato)NiII coordination compound undergoes trimerization when its powder experiences even a single ball impact. Based on systematic experiments with individual ball impacts and analysis by Raman spectroscopy, we provide here quantitative mapping of the transformation in the powder compact and deduce bulk reaction kinetics from multiple individual impacts. 相似文献
636.
MAO/CpTiCl3 is an active catalyst for the polymerization of various types of 1,3-dienes. Butadiene, (E) - and (Z) −1,3-pentadiene, (E) −2-methyl-1,3-pentadiene and 2,3-dimethylbutadiene yield, at room temperature, polymers with a cis-1,4 or a mixed cis/1,2 structure. 4-Methyl-1,3-pentadiene and (E,E) −2,4-hexadiene give, respectively, a 1,2 syndiotactic and a trans-1,4/1,2 polymer. MAO/CpTiCl2·2THF and MAO/(CpTiCl2)n are less active than the CpTiCl3 catalyst, but give the same type of polymers. A change of stereospecificity with temperature was observed in the polymerization of (Z)-1,3-pentadiene: a cis-1,4 isotactic polymer was obtained at +20°C, and a crystalline 1,2 syndiotactic polymer at −20°C. This effect was attributed to a different mode of coordination of the monomer, which is cis-η4 at +20°C and may be trans-η2 at −20°C. Results obtained with catalysts from CpTi(OBu)3 and Ti(OBu)4 are reported for comparison. An interpretation is given of the formation of cis-1,4 isotactic poly(2-methylpentadiene) and of 1,2 syndiotactic poly(4-methylpentadiene), as well as of syndiotactic polystyrene. 相似文献
637.
638.
639.
Subeesh Madayanad Suresh Le Zhang David Hall Changfeng Si Gaetano Ricci Tomas Matulaitis Alexandra M. Z. Slawin Stuart Warriner Yoann Olivier Ifor D. W. Samuel Eli Zysman-Colman 《Angewandte Chemie (International ed. in English)》2023,62(8):e202215522
We present a p- and n-doped nonacene compound, NOBNacene, that represents a rare example of a linearly extended ladder-type multiresonant thermally activated delayed fluorescence (MR-TADF) emitter. This compound shows efficient narrow deep blue emission, with a λPL of 410 nm, full width at half maximum, FWHM, of 38 nm, photoluminescence quantum yield, ΦPL of 71 %, and a delayed lifetime, τd of 1.18 ms in 1.5 wt % TSPO1 thin film. The organic light-emitting diode (OLED) using this compound as the emitter shows a comparable electroluminescence spectrum peaked at 409 nm (FWHM=37 nm) and a maximum external quantum efficiency (EQEmax) of 8.5 % at Commission Internationale de l’Éclairage (CIE) coordinates of (0.173, 0.055). The EQEmax values were increased to 11.2 % at 3 wt % doping of the emitter within the emissive layer of the device. At this concentration, the electroluminescence spectrum broadened slightly, leading to CIE coordinates of (0.176, 0.068). 相似文献
640.