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31.
Construction of a New Class of Tetracycline Lead Structures with Potent Antibacterial Activity through Biosynthetic Engineering 下载免费PDF全文
Dr. Urška Lešnik Dr. Tadeja Lukežič Dr. Ajda Podgoršek Dr. Jaka Horvat Dr. Tomaž Polak Dr. Martin Šala Branko Jenko Dr. Kirsten Harmrolfs Dr. Alain Ocampo‐Sosa Prof. Dr. Luis Martínez‐Martínez Dr. Paul R. Herron Dr. Štefan Fujs Dr. Gregor Kosec Prof. Dr. Iain S. Hunter Prof. Dr. Rolf Müller Prof. Dr. Hrvoje Petković 《Angewandte Chemie (International ed. in English)》2015,54(13):3937-3940
Antimicrobial resistance and the shortage of novel antibiotics have led to an urgent need for new antibacterial drug leads. Several existing natural product scaffolds (including chelocardins) have not been developed because their suboptimal pharmacological properties could not be addressed at the time. It is demonstrated here that reviving such compounds through the application of biosynthetic engineering can deliver novel drug candidates. Through a rational approach, the carboxamido moiety of tetracyclines (an important structural feature for their bioactivity) was introduced into the chelocardins, which are atypical tetracyclines with an unknown mode of action. A broad‐spectrum antibiotic lead was generated with significantly improved activity, including against all Gram‐negative pathogens of the ESKAPE panel. Since the lead structure is also amenable to further chemical modification, it is a platform for further development through medicinal chemistry and genetic engineering. 相似文献
32.
Elizabeth Elacqua Maria Gregor 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(28):9627-9632
Reported are well‐defined donor‐acceptor alternating copolymers prepared using ring‐opening metathesis polymerization (ROMP). Unsymmetrical cyclophanedienes comprising electron‐donating (4‐methoxy‐1‐(2‐ethylhexyl)oxy)benzene (MEH) and electron‐accepting benzothiadiazole (BT) rings were synthesized from the corresponding [3.3]dithiaparacyclophanes. ROMP of the strained unsymmetrical and “electronically‐ambiguous” cyclophanedienes proceeded in a controlled manner in the presence of either Hoveyda–Grubbs II or Grubbs II initiator in wake of both steric and electronic encumbrance. The resulting polymers, comprising alternating BT and MEH‐PPV units, are achieved in molecular weights exceeding 20k with ? values ranging from 1.1–1.4. The living nature of the polymerization is verified through the formation of rod‐coil and rod‐rod block copolymers. Our strategy to develop previously unrealized polymers from functional building blocks featuring a locked‐in D‐A unit is significant in a field striving to achieve well‐defined and sequence‐specific materials. 相似文献
33.
Andrea D. Beck David G. Flad Claudia Tonhäuser Gregor Gassner Claus-Dieter Munz 《Flow, Turbulence and Combustion》2016,97(2):475-511
In this work we investigate the interplay of polynomial de-aliasing and sub-grid scale models for large eddy simulations based on discontinuous Galerkin discretizations. It is known that stability is a major concern when simulating underresolved turbulent flows with high order nodal collocation type discretizations. By changing the interpolatory character of the nodal collocation type discretization to a projection based discretization by increasing the number of quadrature points (polynomial de-aliasing), one is able to remove the aliasing induced stability problems. We focus on this effect and on the consequence for large eddy simulations with explicit subgrid scale models. Often, subgrid scale models have to achieve two possibly conflicting tasks in a single simulation: firstly stabilizing the numerics and secondly modeling the physical effect of the missing scales. Within a discontinuous Galerkin approach, it is possible to use either a fast (but potentially aliasing afflicted) nodal collocation discretization or a projection-based (but computationally costly) variant in combination with an explicit subgrid scale model. We use this framework to investigate the effect on the appropriate model parameter of a standard Smagorinsky subgrid scale model and of a Variational Multiscale Smagorinsky formulation. For this we first consider the 3-D viscous Taylor-Green vortex example to investigate the impact on the stability of the method and second the turbulent flow past a circular cylinder to investigate and compare the accuracy of the results. We show that the aliasing instabilities of collocative discretizations severely limit the choice of the model constant, in particular for high order schemes, while for de-aliased DG schemes, the closure model parameters can be chosen independently from the numerical scheme. For the cylinder flow, we also find that for the same model settings, the projection-based results are in better agreement with the reference DNS than those of the collocative scheme. 相似文献
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Orbital angular momentum entangled photons emitted by a down-conversion source are in higher dimensional entangled states. Here we report the experimental confirmation by demonstrating a violation of a generalized Clauser-Horne-Shimony-Holt-type Bell inequality in three dimensions by more than 18 standard deviations. Higher dimensional entangled states allow the realization of new types of quantum communication protocols. They also provide a more secure quantum cryptography scheme. Therefore our experimental results are likely to have applications in future quantum communication technology. 相似文献
38.
Details are given of a selective negative-ion mass-spectrometric method appropriate for the ultratrace determination of metals and organic compounds by means of their complexes. Direct introduction of the sample into the ion-source, attachment of low-energy electrons, and selected-ion monitoring are described, and comparative data are given relating to surface effects at the tips of insertion-probes on detection limits. Detection limits for chromium and cobalt, determined as their tris(2,2,6,6-tetramethylheptane-3,5-dione) chelates, were respectively 1.0 and 0.16 pg, and that for nickel [as its bis(N,N-diethyldithiocarbamate) complex] was 1.0 pg. Detection limits of 2.0 and 1.0 ng are attainable for malathion and ethion by measurement of the nickel(II) complexes of their O,O'-dialkyldithiophosphate hydrolysis products. 相似文献
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Morfill GE Rubin-Zuzic M Rothermel H Ivlev AV Klumov BA Thomas HM Konopka U Steinberg V 《Physical review letters》2004,92(17):175004
Fluid flow around an obstacle was observed at the kinetic (individual particle) level using "complex (dusty) plasmas" in their liquid state. These "liquid plasmas" have bulk properties similar to water (e.g., viscosity), and a comparison in terms of similarity parameters suggests that they can provide a unique tool to model classical fluids. This allows us to study "nanofluidics" at the most elementary-the particle-level, including the transition from fluid behavior to purely kinetic transport. In this (first) experimental investigation we describe the kinetic flow topology, discuss our observations in terms of fluid theories, and follow this up with numerical simulations. 相似文献