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1.
Pengjin Qin Li-An Wang Prof. Joseph M. O'Connor Prof. Kim K. Baldridge Yifan Li Burak Tufekci Jiyue Chen Prof. Arnold L. Rheingold 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(41):18114-18121
Triene 6π electrocyclization, wherein a conjugated triene undergoes a concerted stereospecific cycloisomerization to a cyclohexadiene, is a reaction of great historical and practical significance. In order to circumvent limitations imposed by the normally harsh reaction conditions, chemists have long sought to develop catalytic variants based upon the activating power of metal–alkene coordination. Herein, we demonstrate the first successful implementation of such a strategy by utilizing [(C5H5)Ru(NCMe)3]PF6 as a precatalyst for the disrotatory 6π electrocyclization of highly substituted trienes that are resistant to thermal cyclization. Mechanistic and computational studies implicate hexahapto transition-metal coordination as responsible for lowering the energetic barrier to ring closure. This work establishes a foundation for the development of new catalysts for stereoselective electrocyclizations. 相似文献
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It is known that a distance-regular graph with valency k at least three admits at most two Qpolynomial structures. We show that all distance-regular graphs with diameter four and valency at least three admitting two Q-polynomial structures are either dual bipartite or almost dual bipartite. By the work of Dickie(1995) this implies that any distance-regular graph with diameter d at least four and valency at least three admitting two Q-polynomial structures is, provided it is not a Hadamard graph, either the cube H(d, 2)with d even, the half cube 1/2H(2d + 1, 2), the folded cube?H(2d + 1, 2), or the dual polar graph on [2A2d-1(q)]with q 2 a prime power. 相似文献
4.
Stuart P. RomerilVictor Lee Jack E. Baldwin Timothy D.W. ClaridgeBarbara Odell 《Tetrahedron letters》2003,44(42):7757-7761
The absolute configuration of the marine sponge alkaloid pyrinodemin A is established by organic synthesis. 相似文献
5.
Jack Harrowfield Dominique Matt 《Journal of inclusion phenomena and macrocyclic chemistry》2004,50(3-4):133-150
The problems involved in identifying and quantifying labile interactions considered to influence complex compound structures are highlighted through the assessment of four different families of metal complexes for which extensive crystallographic data are available. Modification of the charge distribution within a ligand molecule as a result of coordination is one factor with a number of ramifications. A detailed analysis of evidence for both intra- and inter-molecular attractions in dimethylsulfoxide complexes of metal perchlorates is used to provide a basis for the consideration of weak interactions between complex ions involving forces including phenyl-group attractions, hydrogen bonding and cavity inclusion. 相似文献
6.
LetBr(K) denote the Brauer group of a fieldK andPS(K) the projective Schur subgroup.
1. LetK be a finitely generated infinite field. ThenPS(K)=Br(K) if and only ifK is a global field.
2.|LetK be a finitely generated infinite field, and letK((t)) denote the field of formal power series int overK. ThenPS(K((t)))=Br(K((t))) if and only ifK=ℚ. 相似文献
7.
The results of Monte Carlo simulations of the beta dose rate to enamel are presented. The dose rates are the most comprehensive to date, incorporating the beta spectrum from 21 different radionuclides, all internal conversion and Auger electrons, the majority of the bremsstrahlung radiation, effects due to radon loss in the uranium series, and variations in the moisture content of the sediment. Applications to a new dating technique in archaeology using electron spin resonance and beta-gradient isochrons are discussed. 相似文献
8.
We apply a Bayesian approach to the problem of prediction in an unbalanced growth curve model using noninformative priors. Due to the complexity of the model, no analytic forms of the predictive densities are available. We propose both approximations and a prediction-oriented Metropolis-Hastings sampling algorithm for two types of prediction, namely the prediction of future observations for a new subject and the prediction of future values for a partially observed subject. They are illustrated and compared through real data and simulation studies. Two of the approximations compare favorably with the approximation in Fearn (1975, Biometrika, 62, 89–100) and are very comparable to the more accurate Rao-Blackwellization from Metropolis-Hastings sampling algorithm. 相似文献
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This paper models a decision where a player must allocate limitedenergy over a contest of uncertain length. The motivating exampleis a squash match where one of the players is not as fit asthe other. Should a player's energy be concentrated in the earlygames of the match? Should it be spread evenly over all possiblegames? Or should it be conserved for the end of the match? Wemodel this as a decision problem where, in each game, the decision-makermust determine how much energy to expend. We assume that thereare only a small number of discrete energy choices for eachgame and that the more energy the decision-maker expends, themore likely he is to win that game. We solve for the optimaldecision with dynamic programming. With only two possible energychoices for each game, we show that it does not matter how energyis expended. In the case where there are three or more energychoices, we show how to take advantage of the structure of theproblem to determine the optimal sequence of decisions. As forpractical advice, the model suggests that when the decision-makerfalls behind in a match, he ought to switch to a more conservativeapproach by dividing his remaining energy evenly among all thepossible remaining games.
Received 14 May 2003. Revised 5 January 2004. 相似文献