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41.
Alem N Yazyev OV Kisielowski C Denes P Dahmen U Hartel P Haider M Bischoff M Jiang B Louie SG Zettl A 《Physical review letters》2011,106(12):126102
Crystalline systems often lower their energy by atom displacements from regular high-symmetry lattice sites. We demonstrate that such symmetry lowering distortions can be visualized by ultrahigh resolution transmission electron microscopy even at single point defects. Experimental investigation of structural distortions at the monovacancy defects in suspended bilayers of hexagonal boron nitride (h-BN) accompanied by first-principles calculations reveals a characteristic charge-induced pm symmetry configuration of boron vacancies. This symmetry breaking is caused by interlayer bond reconstruction across the bilayer h-BN at the negatively charged boron vacancy defects and results in local membrane bending at the defect site. This study confirms that boron vacancies are dominantly present in the h-BN membrane. 相似文献
42.
Akin to the mathematical recreations, John Wilkins' Mathematicall Magick ( 1648) elaborates the pleasant, useful and wondrous part of practical mathematics, dealing in particular with its material culture of machines and instruments. We contextualize the Mathematicall Magick by studying its institutional setting and its place within changing conceptions of art, nature, religion and mathematics. We devote special attention to the way Wilkins inscribes mechanical innovations within a discourse of wonder. Instead of treating ‘wonder’ as a monolithic category, we present a typology, showing that wonders were not only recreative, but were meant to inspire Wilkins' readers to new mathematical inventions. 相似文献
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An impulsive plane wave traverses a stratified medium consisting of a large number N of homogeneous isotropic perfectly elastic layers. The directly transmitted wave is greatly reduced by the cumulative effect of scattering loss at each of the many interfaces. However, close to the arrival of the direct wave is a broad pulse, arising from multiple scattering; this pulse does not decay as rapidly as the direct wave and ultimately appears to diffuse about a moving center. The latter process, which is determined by the medium statistics, leads to time delays, effective anisotropy, and apparent attenuation.
The present work may be regarded as an extension of that described by Burridge, White and Papanicolaou (1988) and Burridge and Chang (1989) to allow for tunneling P waves for S-wave incidence beyond the critical angle.
When the reflection coefficients at the interfaces are scaled as 1/√N while N → ∞, and when time is measured in units of vertical travel time across an average layer, numerical solutions of the exact problem show that the shape of the broad transmitted pulse approaches the limiting form given as the solution of a certain integrodifferential equation in accordance with our asymptotic theory. 相似文献
46.
Inside Back Cover: Designed Enclosure Enables Guest Binding Within the 4200 Å3 Cavity of a Self‐Assembled Cube (Angew. Chem. Int. Ed. 19/2015) 下载免费PDF全文
47.
Six‐Coordinate Group 13 Complexes: The Role of d Orbitals and Electron‐Rich Multi‐Center Bonding 下载免费PDF全文
Maarten G. Goesten Dr. Célia Fonseca Guerra Prof. Dr. Freek Kapteijn Prof. Dr. Jorge Gascon Prof. Dr. F. Matthias Bickelhaupt 《Angewandte Chemie (International ed. in English)》2015,54(41):12034-12038
Bonding in six‐coordinate complexes based on Group 13 elements (B, Al, Ga, In, Tl) is usually considered to be identical to that in transition‐metal analogues. We herein demonstrate through sophisticated electronic‐structure analyses that the bonding in these Group 13 element complexes is fundamentally different and better characterized as electron‐rich hypervalent bonding with essentially no role for the d orbitals. This characteristic is carried through to the molecular properties of the complex. 相似文献
48.
High‐Resolution Single‐Molecule Fluorescence Imaging of Zeolite Aggregates within Real‐Life Fluid Catalytic Cracking Particles 下载免费PDF全文
Zoran Ristanović Dr. Marleen M. Kerssens Alexey V. Kubarev Frank C. Hendriks Dr. Peter Dedecker Prof. Dr. Johan Hofkens Prof. Dr. Maarten B. J. Roeffaers Prof. Dr. Bert M. Weckhuysen 《Angewandte Chemie (International ed. in English)》2015,54(6):1836-1840
Fluid catalytic cracking (FCC) is a major process in oil refineries to produce gasoline and base chemicals from crude oil fractions. The spatial distribution and acidity of zeolite aggregates embedded within the 50–150 μm‐sized FCC spheres heavily influence their catalytic performance. Single‐molecule fluorescence‐based imaging methods, namely nanometer accuracy by stochastic chemical reactions (NASCA) and super‐resolution optical fluctuation imaging (SOFI) were used to study the catalytic activity of sub‐micrometer zeolite ZSM‐5 domains within real‐life FCC catalyst particles. The formation of fluorescent product molecules taking place at Brønsted acid sites was monitored with single turnover sensitivity and high spatiotemporal resolution, providing detailed insight in dispersion and catalytic activity of zeolite ZSM‐5 aggregates. The results point towards substantial differences in turnover frequencies between the zeolite aggregates, revealing significant intraparticle heterogeneities in Brønsted reactivity. 相似文献
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Improved Spectral Coverage and Fluorescence Quenching in Donor–acceptor Systems Involving Indolo[3‐2‐b]carbazole and Boron‐dipyrromethene or Diketopyrrolopyrrole 下载免费PDF全文
Adis Khetubol Sven Van Snick Melissa L. Clark Eduard Fron Eduardo Coutiño‐González Arvid Cloet Koen Kennes Yuliar Firdaus Maarten Vlasselaer Volker Leen Wim Dehaen Mark Van der Auweraer 《Photochemistry and photobiology》2015,91(3):637-653
A novel π‐conjugated triad and a polymer incorporating indolo[3,2‐b]‐carbazole (ICZ) and 4,4‐difluoro‐4‐bora‐3a,4a‐diaza‐s‐indacene (BODIPY) were synthesized via a Sonogashira coupling. Compared to the parent BODIPY the absorption and fluorescence spectrum were for both compounds broader and redshifted. The redshift of the fluorescence and the decrease of the fluorescence quantum yield and decay time upon increasing solvent polarity were attributed to the formation of a partial charge‐transfer state. Upon excitation in the ICZ absorption band the ICZ fluorescence was quenched in both compounds mainly due to energy transfer to the BODIPY moiety. In a similar ICZ–π–DPP polymer (where DPP is diketopyrrolopyrrole), a smaller redshift of the absorption and fluorescence spectra compared to the parent DPP was observed. A less efficient quenching of the ICZ fluorescence in the ICZ–π–DPP polymer could be related to the unfavorable orientation of the transition dipoles of ICZ and DPP. The rate constant for energy transfer was for all compounds an order of magnitude smaller than predicted by Förster theory. While in a solid film of the triad a further redshift of the absorption maximum of nearly 100 nm was observed, no such shift was observed for the ICZ–π–BODIPY polymer. 相似文献
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