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21.
William K. Bell Brandon M. Rawlings Brian K. Long R. Chad Webb B. Keith Keitz Lukas Häußling C. Grant Willson 《Journal of polymer science. Part A, Polymer chemistry》2014,52(19):2769-2775
A series of photocrosslinkable polymers bearing hyperpolarizable side chain chromophores was synthesized, poled and evaluated on the basis of the thermal stability of Second Harmonic Generation (SHG). Photoinitiation allowed for control of the onset of curing. Crosslinking was monitored by infrared spectroscopy and optimal conversion was achieved by applying a slow temperature ramp during exposure. The ultimate stability of the poled polymers was directly related to the number of crosslinking substituents that were attached to the chromophore pendant group. With two reactive groups per chromophore significant SHG was retained at temperatures above the initial polymer glass transition temperature. © 2014 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2014 , 52, 2769–2775 相似文献
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Xu‐Wen Li Alexandre Ear Lukas Roger Dr. Nassima Riache Alexandre Deville Dr. Bastien Nay 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(48):16389-16393
A bio‐inspired strategy was used to complete the formal synthesis of the antitubercular hirsutellone B and congeners A and C, through construction of its decahydrofluorene core from a linear polyene strand activated at both ends by a silyl enol ether and an allyl acetate. Our synthesis features a key electrophilic cyclization, starting with the remote activation (by [Yb(OTf)3] or BF3 ? OEt2) of the allyl acetate and stereoselectively affording the C ring. This was followed by an intramolecular Diels–Alder reaction to get the tricyclic core of the natural product. The stereoselective reduction of the resulting ketone towards the formal intermediate was critical to the success of this strategy. 相似文献
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Lukas Lohmeyer Dr. Elisabeth Kaifer Prof. Hubert Wadepohl Prof. Hans-Jörg Himmel 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(26):5834-5845
New redox-active 1,2,5,6-tetrakis(guanidino)-naphthalene compounds, isolable and storable in the neutral and deep-green dicationic redox states and oxidisable further in two one-electron steps to the tetracations, are reported. Protonation switches on blue fluorescence, with the fluorescence intensity (quantum yield) increasing with the degree of protonation. Reactions with N-halogenosuccinimides or N-halogenophthalimides led to a series of new redox-active halogeno- and succinimido-/phthalimido-substituted derivatives. These highly selective reactions are proposed to proceed via the tri- or tetracationic state as the intermediate. The derivatives are oxidised reversibly at slightly higher potentials than that of the unsubstituted compounds to dications and further to tri- and tetracations. The integration of redox-active ligands in the transition-metal complexes shifts the redox potentials to higher values and also allows reversible oxidation in two potentially separated one-electron steps. 相似文献
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Dr. Lukas Kaltschnee Dr. Anil P. Jagtap Dr. Jeffrey McCormick Dr. Shawn Wagner Prof. Dr. Louis-S. Bouchard Prof. Dr. Marcel Utz Prof. Dr. Christian Griesinger Dr. Stefan Glöggler 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(47):11031-11035
NMR offers many possibilities in chemical analysis, structural investigations, and medical diagnostics. Although it is broadly used, one of NMR spectroscopies main drawbacks is low sensitivity. Hyperpolarization techniques enhance NMR signals by more than four orders of magnitude allowing the design of new contrast agents. Parahydrogen induced polarization that utilizes the para-hydrogen's singlet state to create enhanced signals is of particular interest since it allows to produce molecular imaging agents within seconds. Herein, we present a strategy for signal enhancement of the carbonyl 13C in amino acids by using parahydrogen, as demonstrated for glycine and alanine. Importantly, the hyperpolarization step is carried out in water and chemically unmodified canonical amino acids are obtained. Our approach thus offers a high degree of biocompatibility, which is crucial for further application. The rapid sample hyperpolarization (within seconds) may enable the continuous production of biologically useful probes, such as metabolic contrast agents or probes for structural biology. 相似文献
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Lukas Meier Christian Berchtold Stefan Schmid Renato Zenobi 《Journal of mass spectrometry : JMS》2012,47(5):555-559
In this study, we use an ion funnel (IF) at ambient pressure to enhance the sensitivity of secondary electrospray ionization (SESI). Atenolol, salbutamol and cocaine as test compounds are delivered to the SESI interface in the gas phase and are charged with three nano electrosprays. In our experiments, we show that the compounds can be detected at concentrations in the low pptv range, which is an increase of two orders of magnitude compared with the results without the IF. With a standard SESI interface, the compounds could not be detected at all. With the use of the SESI IF interface for the headspace analysis of bananas and limes, we can detect many more compounds and at higher intensities than with a standard SESI interface. Copyright © 2012 John Wiley & Sons, Ltd. 相似文献
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Hydrogels have gained importance during the last years due to their wide range of synthetically fabricable elastic properties as well their increasing meaning in biomedical applications. Future exploitation of the vast prospects of hydrogels is however only feasible by establishing reliable material models that precisely capture their behavior in different environments. To this end, we propose a consistent variational framework for deformation-diffusion processes, offering a canonically compact approach to the chemo-mechanical coupling of hydrogels via a saddle-point as well as a new minimization formulation. The work depicts the construction of rate-type potentials for the chemo-mechanical evolution problem and their transformation into time-discrete incremental potentials. In terms of spatial discretization, the finite element method is employed, benefiting from the intrinsic symmetric structure of the variational foundation. While the saddle-point formulation yields the well-known LBB condition as a constraint for finite element interpolations, on the part of its minimizing counterpart H(Div, ℬ︁)-conforming elements have to be chosen. We illustrate appropriate solutions to both challenges, using mixed Taylor-Hood for the saddle-point and Raviart-Thomas elements for the minimization formulation and discuss advantages of the new approach. (© 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献