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Shyjumon Ibrahimkutty Daniel Issenmann Stefan Schleef Anke‐Susanne Müller Yves‐Laurent Mathis Biliana Gasharova Erhart Huttel Ralph Steininger Jörg Göttlicher Tilo Baumbach Albrecht Bartels Christof Janke Anton Plech 《Journal of synchrotron radiation》2011,18(4):539-545
A high‐repetition‐rate pump–probe experiment is presented, based on the asynchronous sampling approach. The low‐α mode at the synchrotron ANKA can be used for a time resolution down to the picosecond limit for the time‐domain sampling of the coherent THz emission as well as for hard X‐ray pump–probe experiments, which probe structural dynamics in the condensed phase. It is shown that a synchronization of better than 1 ps is achieved, and examples of phonon dynamics of semiconductors are presented. 相似文献
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Sebastian Schlund Eline M. Basílio Janke Klaus Weisz Bernd Engels 《Journal of computational chemistry》2010,31(4):665-670
This study investigates how the various components (method, basis set, and treatment of solvent effects) of a theoretical approach influence the relative energies between keto and enol forms of acetylacetone, which is an important model system to study the solvent effects on chemical equilibria from experiment and theory. The computations show that the most popular density functional theory (DFT) approaches, such as B3LYP overestimate the stability of the enol form with respect to the keto form by ~10 kJ mol?1, whereas the very promising SCS‐MP2 approach is underestimating it. MP2 calculations indicate that in particular the basis set size is crucial. The Dunning Huzinaga double ζ basis (D95z(d,p)) used in previous studies overestimates the stability of the keto form considerably as does the popular split‐valence plus polarization (SVP) basis. Bulk properties of the solvent included by continuum approaches strongly stabilize the keto form, but they are not sufficient to reproduce the reversal in stabilities measured by low‐temperature nuclear magnetic resonance experiments in freonic solvents. Enthalpic and entropic effects further stabilize the keto form, however, the reversal is only obtained if also molecular effects are taken into account. Such molecular effects seem to influence only the energy difference between the keto and the enol forms. Trends arising due to variation in the dielectric constant of the solvent result from bulk properties of the solvent, i.e., are already nicely described by continuum approaches. As such this study delivers a deep insight into the abilities of various approaches to describe solvent effects on chemical equilibria. © 2009 Wiley Periodicals, Inc. J Comput Chem, 2010 相似文献
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Jennifer E. Mihalick William P. Griffiths III James E. Muten Travis A. Olson John B. Hein 《Journal of solution chemistry》1999,28(8):1019-1030
Solution calorimetry was used to determine enthalpies and stability constants for binding of lead(II) or cadmium(II) by galacturonic acid and several monosaccharides in aqueous solution. New values for enthalpies of solution in water are reported for galacturonic acid and maltose monohydrate. The interaction of water solvent with the reactants is the largest factor in the binding process. 相似文献
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Two femtosecond Ti:sapphire lasers with slightly different repetition rates near 1 GHz are coupled to implement high-speed asynchronous optical sampling. The application of this technique is successfully demonstrated in the field of terahertz time-domain spectroscopy (TDS). A time delay of 1 ns is scanned at a frequency of 5 kHz without moving mechanical parts. Compared with that of conventional TDS schemes based on lock-in detection and moving mirrors, the readout time of integrated resonant THz sensors is reduced by a factor of 20, opening the way for high-throughput THz sensing in marker-free DNA analysis. 相似文献
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Unprecedented optical control of the surface plasmon polariton assisted transmission of terahertz radiation through subwavelength apertures is rendered possible by carrier-induced changes to the dielectric properties of a semiconductor grating. Although the study presented is static, the extension of our approach to dynamic switching and tuning is deemed straightforward, opening the way for the realization of ultrafast surface plasmon based devices. 相似文献
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Bragg gratings are used in several photonic devices to reflect, and thus to isolate, specific wavelengths of light. Gratings can be photoinduced in chalcogenide glasses by illumination of bandgap light in an interference pattern. We used holographic interferometry to create Bragg gratings in amorphous As2Se3 thin films with a period of 0.56 microm by illumination with 633-nm light. The quality of the gratings was tested in real time, and refractive-index modulations as high as 0.037 were measured. These gratings were found to be stable over a period of several months if they were kept in the dark. 相似文献
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We present a temperature-independent Monte Carlo method for the determination of the density of states of lattice proteins that combines the fast ground-state search strategy of the new pruned-enriched Rosenbluth chain-growth method and multicanonical reweighting for sampling the complete energy space. Since the density of states contains all energetic information of a statistical system, we can directly calculate the mean energy, specific heat, Helmholtz free energy, and entropy for all temperatures. We apply this method to lattice proteins consisting of hydrophobic and polar monomers, and for the examples of sequences considered, we identify the transitions between native, globule, and random coil states. Since no special properties of heteropolymers are involved in this algorithm, the method applies to polymer models as well. 相似文献