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981.
982.
The different mechanisms, rotation, inversion, or intermediate mechanism, by which occur the topomerization of imine systems R2 CN X have been studied by applying ab initio, B3LYP, and MP2 methods. The effect of a wide variety of substituents R and X on the isomerization pathway have been examined by computing fully optimized structures of the ground and transition states (136 isomers belonging to different imine families were studied and more than 300 transition structures were determined at various levels of theory). Energy barriers have been also obtained and it was found that the groups R and X have a strong influence on the type of mechanism involved and the activation energies. Thus, and depending on the type of substituents, transition state structures related to the following kinds of processes were found: pure inversion, intermediate mechanisms, rotation, and enhanced rotation (hyper‐rotation). In turn, the corresponding activation energies range between very low (<10 kcal/mol) and extremely high (> 70 kcal/mol) values. A simple index that allows us to quantify the percentage of inversion or rotation mechanism is proposed. © 2009 Wiley Periodicals, Inc. J Comput Chem, 2010 相似文献
983.
For an accurate simulation of forming processes, it is of paramount importance to model the different lubrication regimes that can develop at the contact interface. These might vary from zone to zone of the forming piece, and from one regime to another, resulting in forces of different nature and magnitude. In these cases, the use of the classical Coulomb friction law will be clearly not sufficient to capture, in a suitable manner, the variety of forces applied on the forming piece. 相似文献
984.
Miguel Martín 《Mathematische Nachrichten》2008,281(3):376-385
A Banach space X is said to have the alternative Daugavet property if for every (bounded and linear) rank‐one operator T: X → X there exists a modulus one scalar ω such that ∥Id+ωT ∥ = 1 + ∥T ∥. We give geometric characterizations of this property in the setting of C *‐algebras, JB *‐triples, and of their isometric preduals. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim) 相似文献
985.
Graciela Martínez‐Paredes María Begoña González‐García Agustín Costa‐García 《Electroanalysis》2009,21(8):925-930
Gold nanostructured screen‐printed carbon electrodes are demonstrated to be suitable transducers for the determination of lead using square‐wave voltammetry. Reproducible gold nanostructures have been obtained by direct electrochemical deposition. A calibration plot from 2.5 to 250 μg/L was obtained in acidic solutions of Pb(II) with a reproducibility of 4% (n=10). The detection limit was 0.09 μg/L of lead. The method is then applied to perform a blood lead analysis by adjusting square‐wave parameters in capillary or venous blood with a minimum sample pretreatment and excellent accuracy and reproducibility. 相似文献
986.
987.
988.
Antonio Herrera Nazario Martín Rachid Chioua Ángel Sánchez-Vázquez John Almy 《Tetrahedron》2009,65(8):1697-2715
Two alternative methods for the preparation of new pyrimidine Diels-Alder cycloadducts from the readily available 2,4-bis(methylsulfanyl)-5,6-dihydrocyclobuta[d]pyrimidine are presented. In the first method, the in situ generated pyrimidine ortho-quinodimethane reacts with various dienophiles to form the respective cycloadducts bearing two methylthio groups, which can be easily replaced by other functional groups. In the second method, one or both of the methylsulfanyl groups of the starting pyrimidine are replaced first and the resulting functionalized pyrimidines are able to undergo Diels-Alder cyclization with different dienophiles to form pyrimidine cycloadducts. These alternative synthetic strategies provide access to a wide variety of pyrimidine cycloadducts with a different substitution pattern on the pyrimidine ring. Yield data indicate that the electronic nature of the functional groups strongly influence the efficiency of the cycloaddition reaction. 相似文献
989.
990.
R. Andreani E. G. Birgin J. M. Martínez M. L. Schuverdt 《Mathematical Programming》2008,111(1-2):5-32
Two Augmented Lagrangian algorithms for solving KKT systems are introduced. The algorithms differ in the way in which penalty
parameters are updated. Possibly infeasible accumulation points are characterized. It is proved that feasible limit points
that satisfy the Constant Positive Linear Dependence constraint qualification are KKT solutions. Boundedness of the penalty
parameters is proved under suitable assumptions. Numerical experiments are presented.
The authors were supported by PRONEX - CNPq / FAPERJ E-26 / 171.164/2003 - APQ1, FAPESP (Grants 2001/04597-4, 2002/00094-0,
2003/09169-6, 2002/00832-1 and 2005/56773-1) and CNPq. 相似文献