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111.
Etienne Plésiat Piero Decleva Fernando Martín 《Central European Journal of Physics》2013,11(9):1157-1162
We use an extension of the static-exchange density functional theory (DFT) method, previously reported in [E. Plésiat et al., Phys. Rev. A 2, 023409 (2012), E. Plésiat, P. Decleva, F. Martín, Phys. Chem. Chem. Phys. 31, 10853 (2012)], to evaluate vibrationally resolved (total and angular) K-shell photoelectron cross sections of methane. The calculated cross sections are in very good agreement with the existing experimental measurements at low photoelectron energies. We show that, in contrast with the rich interference patterns previously observed in molecular frame C(1s) photoelectron angular distributions of methane at both low and high photoelectron energy, no interference effects are observed in the calculated β parameters, even at high photon energies. 相似文献
112.
Etienne Boutin Min Wang John C. Lin Matthieu Mesnage Daniela Mendoza Benedikt Lassalle‐Kaiser Christopher Hahn Thomas F. Jaramillo Marc Robert 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(45):16318-16322
Conversion of CO2 into valuable molecules is a field of intensive investigation with the aim of developing scalable technologies for making fuels using renewable energy sources. While electrochemical reduction into CO and formate are approaching industrial maturity, a current challenge is obtaining more reduced products like methanol. However, literature on the matter is scarce, and even more for the use of molecular catalysts. Here, we demonstrate that cobalt phthalocyanine, a well‐known catalyst for the electrochemical conversion of CO2 to CO, can also catalyze the reaction from CO2 or CO to methanol in aqueous electrolytes at ambient conditions of temperature and pressure. The studies identify formaldehyde as a key intermediate and an unexpected pH effect on selectivity. This paves the way for establishing a sequential process where CO2 is first converted to CO which is subsequently used as a reactant to produce methanol. Under ideal conditions, the reaction shows a global Faradaic efficiency of 19.5 % and chemical selectivity of 7.5 %. 相似文献
113.
Etienne A. Lapierre Prof. Warren E. Piers Jian-Bin Lin Chris Gendy 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(17):4305-4308
Isolable cationic PtII and PtIV alkylidenes, proposed intermediates in catalytic organic transformations, are reported. The bonding in these species was probed by experimental, structural, spectroscopic, electrochemical and computational methods, providing direct evidence for π-bonding, the often-theorized relativistic stabilization of these species, and the influence of oxidation state. 相似文献
114.
115.
Vi Le Etienne Pardoux 《Stochastics An International Journal of Probability and Stochastic Processes》2020,92(6):852-875
Consider a general continuous-state branching process with additional interaction, which destroys the branching property. We give precise conditions on the interaction term, in order to decide whether the extinction time of the process remains or not bounded as the initial value tends to infinity, and similarly for the total mass of the process. 相似文献
116.
P. Etienne P. Coudray Y. Moreau J. Porque 《Journal of Sol-Gel Science and Technology》1998,13(1-3):523-527
The development and characterization of channel waveguides using wet-process, low temperature sol-gel chemistry is described. Two structures have been developed. The first one is a one-layer structure, composed of a sol-gel solution which is a mixture of photopolymerizable organosilicate and organozirconate precursors. The other is a multilayer structure with a buffer under the guide and a protective coating. The layers are deposited by the dipping technique. The devices are obtained by UV light exposure of the coating through a predefined mask (channel waveguides). The refractive index increase is sufficient enough to allow the use of waveguides in the 1.55 m telecommunication window.These waveguides are thick enough to reduce the coupling losses with an optical fiber below 0.5 dB. Also, because of our sandwich structure, the propagation losses are less than 0.1 dB. 相似文献
117.
118.
Here we redesigned the branches of polyamidoamine (PAMAM) dendrimers by moving the amide carbonyl group on the other side of the amide nitrogen atom, transforming the β-alaninyl-amidoethylamine branch, which easily undergoes retro-Michael reactions and renders PAMAMs intrinsically unstable, into a more stable glycyl-amidopropylamine branch. The resulting inverse PAMAM (i-PAMAM) dendrimers have the same carbon framework as PAMAMs and only differ by the position of the carbonyl group. In contrast to PAMAMs which are prepared in solution and are difficult to purify, we synthesize i-PAMAMs using high-temperature solid-phase peptide synthesis by iterative coupling and deprotection of the commercially available N,N-bis(N′-Fmoc-3-aminopropyl)glycine and purify them preparative reverse phase HPLC. Our i-PAMAM dendrimers show no detectable degradation over time. We demonstrate this new class of dendrimers with the synthesis of antimicrobial dendrimers with potent yet non-membrane disruptive activities against both Gram-negative and Gram-positive bacteria. 相似文献
119.
Cho KB Hirao H Chen H Carvajal MA Cohen S Derat E Thiel W Shaik S 《The journal of physical chemistry. A》2008,112(50):13128-13138
This study directly compares the active species of heme enzymes, so-called Compound I (Cpd I), across the heme-thiolate enzyme family. Thus, sixty-four different Cpd I structures are calculated by hybrid quantum mechanical/molecular mechanical (QM/MM) methods using four different cysteine-ligated heme enzymes (P450(cam), the mutant P450(cam)-L358P, CPO and NOS) with varying QM region sizes in two multiplicities each. The overall result is that these Cpd I species are similar to each other with regard to many characteristic features. Hence, using the more stable CPO Cpd I as a model for P450 Cpd I in experiments should be a reasonable approach. However, systematic differences were also observed, and it is shown that NOS stands out in most comparisons. By analyzing the electrical field generated by the enzyme on the QM region, one can see that (a) the protein exerts a large influence and modifies all the Cpd I species compared with the gas-phase situation and (b) in NOS this field is approximately planar to the heme plane, whereas it is approximately perpendicular in the other enzymes, explaining the deviating results on NOS. The calculations on the P450(cam) mutant L358P show that the effects of removing the hydrogen bond between the heme sulfur and L358 are small at the Cpd I stage. Finally, Mossbauer parameters are calculated for the different Cpd I species, enabling future comparisons with experiments. These results are discussed in the broader context of recent findings of Cpd I species that exhibit large variations in the electronic structure due to the presence of the substrate. 相似文献
120.
Stan Alama Lia Bronsard Etienne Sandier 《Transactions of the American Mathematical Society》2008,360(1):1-34
We consider the Lawrence-Doniach model for layered superconductors, in which stacks of parallel superconducting planes are coupled via the Josephson effect. To model experiments in which the superconductor is placed in an external magnetic field oriented parallel to the superconducting planes, we study the structure of isolated vortices for a doubly periodic problem. We consider a singular limit which simulates certain experimental regimes in which isolated vortices have been observed, corresponding to letting the interlayer spacing of the superconducting planes tend to zero and the Ginzburg-Landau parameter simultaneously, but at a fixed relative rate.