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Exciton‐Vibrational Couplings in Homo‐ and Heterodimer Stacks of Perylene Bisimide Dyes within Cyclophanes: Studies on Absorption Properties and Theoretical Analysis
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David Bialas Christoph Brüning Dr. Felix Schlosser Dr. Benjamin Fimmel Johannes Thein Prof. Dr. Volker Engel Prof. Dr. Frank Würthner 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(42):15011-15018
The optical properties of a series of three cyclophanes comprising either identical or different perylene bisimide (PBI) chromophores were studied by UV/Vis absorption spectroscopy and their distinctive spectral features were analyzed. All the investigated cyclophanes show significantly different absorption features with respect to the corresponding constituent PBI monomers indicating strong coupling interactions between the PBI units within the cyclophanes. DFT calculations suggest a π‐stacked arrangement of the PBI units at close van der Waals distance in the cyclophanes with rotational displacement. Simulations of the absorption spectra based on time‐dependent quantum mechanics properly reproduced the experimental spectra, revealing exciton‐vibrational coupling between the chromophores both in homo‐ and heterodimer stacks. The PBI cyclophane comprising two different PBI chromophores represents the first example of a PBI heterodimer stack for which the exciton coupling has been investigated. The quantum dynamics analysis reveals that exciton coupling in heteroaggregates is indeed of similar strength as for homoaggregates. 相似文献
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Flow over a compliant membrane is a complex problem where the interaction between fluid and membrane determines the nature of the aerodynamic characteristics of the membrane wing. This investigation is concerned with the deformation and oscillatory motion of a membrane under aerodynamic loading. The approach is computational, but the analytical solution is also presented for a constant pressure loading. The computational results are compared with the experimental data available in the literature as well as with the present analytical solution. In this study, the values of Reynolds number are 38 416 and 141 500, and the angle of attack and prestrain range from 10° to 40° and from 0 to 0.074, respectively. This range of parameters makes the outcome of the investigation more relevant to applications involving the flight of micro air vehicles and the membrane wings of flying mammals such as bats. The computations indicate a mostly asymmetric deflection with the point of maximum camber located nearly at 40% of the chord length from the leading edge. The deflection is decreased with prestrain, and it is increased with Reynolds number. Moreover, the lift coefficient generally increases with the angle of attack. However, for Re=141 500, it increases first to a peak at 20–30° angle of attack, and then decreases. The drag coefficient is much higher than that of conventional airfoils. The membrane oscillates in the streamwise and vertical directions. The largest amplitude of oscillations is observed at 40° for Re=38 416. The oscillations are caused by the oscillatory nature of the flow due to fluid–membrane interaction and the formation of the leading edge and trailing edge vortices. Compared with a rigid membrane of the same camber, the compliant membrane has a smaller recirculation region which may lead to a delayed stall. 相似文献
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We present a new method for resolving combinatorial ambiguities that arise in multi-particle decay chains at hadron colliders where the assignment of visible particles to the different decay chains has ambiguities. Our method, based on selection cuts favoring high transverse momentum and low invariant mass pairings, is shown to be significantly superior to the more traditional hemisphere method for a large class of decay chains, producing an increase in signal retention of up to a factor of 2. This new method can thus greatly reduce the combinatorial ambiguities of decay chain assignments. 相似文献
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Anzenbacher P Tyson DS Jursíková K Castellano FN 《Journal of the American Chemical Society》2002,124(22):6232-6233
A new Ru(II) complex is described which serves as a luminescence lifetime-based sensor for fluoride and cyanide anions (KF = 640 000 mol-1, KCN = 430 000 mol-1). This chromophore displays observable changes in its UV-vis and steady-state luminescence spectra upon cyanide binding. Prior to cyanide addition, this complex exhibits a single-exponential lifetime (tau = 377 +/- 20 ns). With increasing cyanide concentrations, the intensity decays are composed of two exponentials: long tau (320-370 ns) and short tau (13-17 ns). The average lifetimes shorten as a function of cyanide concentration since the fractional intensity shifts from an initial dominant long lifetime component to the short lifetime component. This work represents the first example of a direct method for the luminescence lifetime-based sensing of anions. 相似文献
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The mutual influence of two layers with strongly localized electrons is exercised though the random Coulomb shifts of site energies in one layer caused by electron hops in the other layer. We trace how these shifts give rise to a voltage drop in the passive layer, when a current is passed through the active layer. We find that the microscopic origin of drag lies in the time correlations of the occupation numbers of the sites involved in a hop. These correlations are neglected within the conventional Miller-Abrahams scheme for calculating the hopping resistance. 相似文献
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