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11.
Hydroxymethylated Phyllobilins: A Puzzling New Feature of the Dioxobilin Branch of Chlorophyll Breakdown
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Iris Süssenbacher Dr. Bastien Christ Prof. Dr. Stefan Hörtensteiner Prof. Dr. Bernhard Kräutler 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(1):87-92
Colorless nonfluorescent chlorophyll (Chl) catabolites (NCCs) are formyloxobilin‐type phyllobilins, which are considered the typical products of Chl breakdown in senescent leaves. However, in degreened leaves of some plants, dioxobilin‐type Chl catabolites (DCCs) predominate, which lack the formyl group of the NCCs, and which arise from Chl catabolites by oxidative removal of the formyl group by a P450 enzyme. Here a structural investigation of the DCCs in the methylesterase16 mutant of Arabidopsis thaliana is reported. Eight new DCCs were identified and characterized structurally. Strikingly, three of these DCCs carry stereospecifically added hydroxymethyl groups, and represent bilin‐type linear tetrapyrroles with an unprecedented modification. Indeed, DCCs show a remarkable structural parallel, otherwise, to the bilins from heme breakdown. 相似文献
12.
Streubel R Schiemann U Jones PG Tran Huy NH Mathey F 《Angewandte Chemie (International ed. in English)》2000,39(20):3686-3688
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The ultrafast dephasing of waveguide-plasmon polaritons in metallic photonic crystal slabs is investigated in the femtosecond regime by second-order nonlinear autocorrelation. We find a drastic modification of the dephasing rates due to interaction between localized particle plasmons and optical waveguide modes and subsequent modification of the photonic density of states. In the strong coupling regime our measurements give clear evidence for the appearance of ultrafast polaritonic beat phenomena. All experimental results agree well with theoretical simulations based on a coupled damped harmonic oscillator model. 相似文献
14.
Clara D. Christ Alan E. Mark Wilfred F. van Gunsteren 《Journal of computational chemistry》2010,31(8):1569-1582
Methods to compute free energy differences between different states of a molecular system are reviewed with the aim of identifying their basic ingredients and their utility when applied in practice to biomolecular systems. A free energy calculation is comprised of three basic components: (i) a suitable model or Hamiltonian, (ii) a sampling protocol with which one can generate a representative ensemble of molecular configurations, and (iii) an estimator of the free energy difference itself. Alternative sampling protocols can be distinguished according to whether one or more states are to be sampled. In cases where only a single state is considered, six alternative techniques could be distinguished: (i) changing the dynamics, (ii) deforming the energy surface, (iii) extending the dimensionality, (iv) perturbing the forces, (v) reducing the number of degrees of freedom, and (vi) multi‐copy approaches. In cases where multiple states are to be sampled, the three primary techniques are staging, importance sampling, and adiabatic decoupling. Estimators of the free energy can be classified as global methods that either count the number of times a given state is sampled or use energy differences. Or, they can be classified as local methods that either make use of the force or are based on transition probabilities. Finally, this overview of the available techniques and how they can be best used in a practical context is aimed at helping the reader choose the most appropriate combination of approaches for the biomolecular system, Hamiltonian and free energy difference of interest. © 2009 Wiley Periodicals, Inc. J Comput Chem, 2010 相似文献
15.
We report the realization of a bright ultrafast type II parametric down-conversion source of twin beams free of any spatiotemporal correlations in a periodically poled KTiOPO4 (PP-KTP) waveguide. From a robust, single-pass setup it emits pulsed two-mode squeezed vacuum states: photon-number entangled pairs of single-mode pulses or, in terms of continuous variables quantum optics, pulsed Einstein-Podolsky-Rosen states in the telecom wavelength regime. We verify the single-mode character of our source by measuring Glauber correlation functions g(2) and demonstrate with a pump energy as low as 75 pJ per pump pulse a mean photon number of 2.5. 相似文献
16.
XU Xiaodong CHEN Xiang LI Kaiyuan LIU Xiaojun CHENG Jianchun Christ Glorieux 《声学学报:英文版》2011,(4):391-397
A laser ultrasonics method is used to characterize the propagation properties of surface wave traveling on the surface of materials with sub-surface defect in 2D.Linear and nonlinear propagation properties of ultrasonics caused by the defects have been detected in experiment. A theoretical model is proposed and used to study the linear and nonlinear properties of ultrasonics caused by the defect.The numerical results indicate that the nonlinear ultrasonic wave will be excited when a finite amplitude ultrasonics propagates on the surface of materials with sub-surface defect.The theoretical analysis confirms that the nonlinear wave is caused by the "clapping"of the interface of defect instead of the mode conversions of ultrasonics. 相似文献
17.
Michael Christ 《偏微分方程通讯》2013,38(3-4):117-204
Hypoellipticity in Gevrey classes Gs is characterized for a simple family of sums of suares of verctor fields satisfying the bracket hypothesis, with analytic coefficients. It is shown that hypoellipticity holds if and only if s is greater than or equal to an optimal exponent that may take on any rational value. 相似文献
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19.
In design optimization and parameter identification, the objective, or response function(s) are typically linked to the actually independent variables through equality constraints, which we will refer to as state equations. Our key assumption is that it is impossible to form and factor the corresponding constraint Jacobian, but one has instead some fixed-point algorithm for computing a feasible state, given any reasonable value of the independent variables. Assuming that this iteration is eventually contractive, we will show how reduced gradients (Jacobians) and Hessians (in other words, the total derivatives) of the response(s) with respect to the independent variables can be obtained via algorithmic, or automatic, differentiation (AD). In our approach the actual application of the so-called reverse, or adjoint differentiation mode is kept local to each iteration step. Consequently, the memory requirement is typically not unduly enlarged. The resulting approximating Lagrange multipliers are used to compute estimates of the reduced function values that can be shown to converge twice as fast as the underlying state space iteration. By a combination with the forward mode of AD, one can also obtain extra-accurate directional derivatives of the reduced functions as well as feasible state space directions and the corresponding reduced or projected Hessians of the Lagrangian. Our approach is verified by test calculations on an aircraft wing with two responses, namely, the lift and drag coefficient, and two variables, namely, the angle of attack and the Mach number. The state is a 2-dimensional flow field defined as solution of the discretized Euler equation under transonic conditions. 相似文献
20.