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Victoria L. Challinor Ryne C. Johnston Paul V. Bernhardt Reginald P. Lehmann Elizabeth H. Krenske James J. De Voss 《Chemical science》2015,6(10):5740-5745
A series of novel sesterterpenes (2–6) have been isolated from the roots of Aletris farinosa and structurally characterized by MS, NMR, and X-ray crystallography in conjunction with computational modeling. Their structures provide new insights into the mechanisms of sesterterpene biosynthesis. Specifically, we propose with support from density functional theory computations that the configuration at a single stereocenter determines the fate of a key tetracyclic carbocationic intermediate, derived from an oxidogeranylfarnesol precursor. Whereas one epimer of the carbocation undergoes H+ elimination to give 6, the other undergoes a spectacular cascade of seven 1,2-methyl and hydride migrations leading to the previously unreported carbon skeleton of 5. Theoretical calculations suggest that the cascade is triggered by substrate preorganization in the enzyme active site. 相似文献
64.
Simone Zanella Dr. Michele Mingozzi Alberto Dal Corso Dr. Roberto Fanelli Dr. Daniela Arosio Prof. Dr. Marco Cosentino Dr. Laura Schembri Dr. Franca Marino Dr. Marta De Zotti Prof. Dr. Fernando Formaggio Dr. Luca Pignataro Prof. Dr. Laura Belvisi Prof. Dr. Umberto Piarulli Prof. Dr. Cesare Gennari 《ChemistryOpen》2015,4(5):633-641
A dual-action ligand targeting both integrin αVβ3 and vascular endothelial growth factor receptors (VEGFRs), was synthesized via conjugation of a cyclic peptidomimetic αVβ3 Arg-Gly-Asp (RGD) ligand with a decapentapeptide. The latter was obtained from a known VEGFR antagonist by acetylation at the Lys13 side chain. Functionalization of the precursor ligands was carried out in solution and in the solid phase, affording two fragments: an alkyne VEGFR ligand and the azide integrin αVβ3 ligand, which were conjugated by click chemistry. Circular dichroism studies confirmed that both the RGD and VEGFR ligand portions of the dual-action compound substantially adopt the biologically active conformation. In vitro binding assays on isolated integrin αVβ3 and VEGFR-1 showed that the dual-action conjugate retains a good level of affinity for both its target receptors, although with one order of magnitude (10/20 times) decrease in potency. The dual-action ligand strongly inhibited the VEGF-induced morphogenesis in Human Umbilical Vein Endothelial Cells (HUVECs). Remarkably, its efficiency in preventing the formation of new blood vessels was similar to that of the original individual ligands, despite the worse affinity towards integrin αVβ3 and VEGFR-1. 相似文献
65.
Anirudra Parajuli Daniel H. Kwak Luca Dalponte Dr. Niina Leikoski Tomas Galica Ugochukwu Umeobika Dr. Laurent Trembleau Andrew Bent Prof. Kaarina Sivonen Matti Wahlsten Dr. Hao Wang Dr. Ermanno Rizzi Prof. Gianluca De Bellis Prof. James Naismith Prof. Marcel Jaspars Prof. Xinyu Liu Dr. Wael Houssen Dr. David Peter Fewer 《Angewandte Chemie (International ed. in English)》2017,56(2):433-433
66.
Dr. Yan Li Dr. Yuk-Chi Chan Bi-Xiang Leong Dr. Yongxin Li Dr. Emma Richards Indu Purushothaman Dr. Susmita De Dr. Pattiyil Parameswaran Dr. Cheuk-Wai So 《Angewandte Chemie (International ed. in English)》2017,56(26):7573-7578
The trapping of a silicon(I) radical with N-heterocyclic carbenes is described. The reaction of the cyclic (alkyl)(amino) carbene [cAACMe] (cAACMe=:C(CMe2)2(CH2)NAr, Ar=2,6-iPr2C6H3) with H2SiI2 in a 3:1 molar ratio in DME afforded a mixture of the separated ion pair [(cAACMe)2Si:.]+I− ( 1 ), which features a cationic cAAC–silicon(I) radical, and [cAACMe−H]+I−. In addition, the reaction of the NHC–iodosilicon(I) dimer [IAr(I)Si:]2 (IAr=:C{N(Ar)CH}2) with 4 equiv of IMe (:C{N(Me)CMe}2), which proceeded through the formation of a silicon(I) radical intermediate, afforded [(IMe)2SiH]+I− ( 2 ) comprising the first NHC–parent-silyliumylidene cation. Its further reaction with fluorobenzene afforded the CAr−H bond activation product [1-F-2-IMe-C6H4]+I− ( 3 ). The isolation of 2 and 3 confirmed the reaction mechanism for the formation of 1 . Compounds 1 – 3 were analyzed by EPR and NMR spectroscopy, DFT calculations, and X-ray crystallography. 相似文献
67.
In a seminal work, Boneh, Sahai and Waters (BSW) [TCC’11] showed that for functional encryption the indistinguishability notion of security (IND-Security) is weaker than simulation-based security (SIM-Security), and that SIM-Security is in general impossible to achieve. This has opened up the door to a plethora of papers showing feasibility and new impossibility results. Nevertheless, the quest for better definitions that (1) overcome the limitations of IND-Security and (2) the known impossibility results, is still open. In this work, we explore the benefits and the limits of using efficient rewinding black-box simulators to argue security. To do so, we introduce a new simulation-based security definition, that we call rewinding simulation-based security (RSIM-Security), that is weaker than the previous ones but it is still sufficiently strong to not meet pathological schemes as it is the case for IND-Security (that is implied by the RSIM). This is achieved by retaining a strong simulation-based flavour but adding more rewinding power to the simulator having care to guarantee that it can not learn more than what the adversary would learn in any run of the experiment. What we found is that for RSIM the BSW impossibility result does not hold and that IND-Security is equivalent to RSIM-Security for attribute-based encryption in the standard model. Nevertheless, we prove that there is a setting where rewinding simulators are of no help. The adversary can put in place a strategy that forces the simulator to rewind continuously. 相似文献
68.
In this article we provide a complete classification of regular partial difference sets in Abelian groups of order \(4p^2\), p an odd prime. It turns out that the known examples are the only examples. These are, up to complements, the trivial examples, the PCP examples, and a sporadic example in \(\mathbb {Z}_2^2\times \mathbb {Z}_3^2\). 相似文献
69.
Roberto?Alicandro Lucia?De?Luca Adriana?Garroni Marcello?PonsiglioneEmail author 《Calculus of Variations and Partial Differential Equations》2017,56(5):148
In Alicandro et al. (J Mech Phys Solids 92:87–104, 2016) a simple discrete scheme for the motion of screw dislocations toward low energy configurations has been proposed. There, a formal limit of such a scheme, as the lattice spacing and the time step tend to zero, has been described. The limiting dynamics agrees with the maximal dissipation criterion introduced in Cermelli and Gurtin (Arch Ration Mech Anal 148, 1999) and predicts motion along the glide directions of the crystal. In this paper, we provide rigorous proofs of the results in [3], and in particular of the passage from the discrete to the continuous dynamics. The proofs are based on \(\Gamma \)-convergence techniques. 相似文献
70.
In recent work, we constructed a new near octagon \(\mathcal {G}\) from certain involutions of the finite simple group \(G_2(4)\) and showed a correspondence between the Suzuki tower of finite simple groups, \(L_3(2)< U_3(3)< J_2< G_2(4) < Suz\), and the tower of near polygons, \(\mathrm {H}(2,1) \subset \mathrm {H}(2)^D \subset \mathsf {HJ} \subset \mathcal {G}\). Here we characterize each of these near polygons (except for the first one) as the unique near polygon of the given order and diameter containing an isometrically embedded copy of the previous near polygon of the tower. In particular, our characterization of the Hall–Janko near octagon \(\mathsf {HJ}\) is similar to an earlier characterization due to Cohen and Tits who proved that it is the unique regular near octagon with parameters (2, 4; 0, 3), but instead of regularity we assume existence of an isometrically embedded dual split Cayley hexagon, \(\mathrm {H}(2)^D\). We also give a complete classification of near hexagons of order (2, 2) and use it to prove the uniqueness result for \(\mathrm {H}(2)^D\). 相似文献