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81.
Two independent computational methods have been used for determination of amide resonance stabilization and amidicities relative to N,N-dimethylacetamide for a wide range of acyclic and cyclic amides. The first method utilizes carbonyl substitution nitrogen atom replacement (COSNAR). The second, new approach involves determination of the difference in amide resonance between N,N-dimethylacetamide and the target amide using an isodesmic trans-amidation process and is calibrated relative to 1-aza-2-adamantanone with zero amidicity and N,N-dimethylacetamide with 100% amidicity. Results indicate excellent coherence between the methods, which must be regarded as more reliable than a recently reported approach to amidicities based upon enthalpies of hydrogenation. Data for acyclic planar and twisted amides are predictable on the basis of the degrees of pyramidalization at nitrogen and twisting about the C-N bonds. Monocyclic lactams are predicted to have amidicities at least as high as N,N-dimethylacetamide, and the β-lactam system is planar with greater amide resonance than that of N,N-dimethylacetamide. Bicyclic penam/em and cepham/em scaffolds lose some amidicity in line with the degree of strain-induced pyramidalization at the bridgehead nitrogen and twist about the amide bond, but the most puckered penem system still retains substantial amidicity equivalent to 73% that of N,N-dimethylacetamide. 相似文献
82.
Vicente Campos Fred Glover Manuel Laguna Rafael Martí 《Journal of Global Optimization》2001,21(4):397-414
Scatter search is a population-based method that has recently been shown to yield promising outcomes for solving combinatorial and nonlinear global optimization problems. Based on formulations originally proposed in the 1960s for combining decision rules and problem constraints, such as in generating surrogate constraints, scatter search uses strategies for combining solution vectors that have proved effective in a variety of problem settings. In this paper, we present a scatter search implementation designed to find high quality solutions for the NP-hard linear ordering problem, which has a significant number of applications in practice. The LOP, for example, is equivalent to the so-called triangulation problem for input-output tables in economics. Our implementation incorporates innovative mechanisms to combine solutions and to create a balance between quality and diversification in the reference set. We also use a tracking process that generates solution statistics disclosing the nature of combinations and the ranks of antecedent solutions that produced the best final solutions. Extensive computational experiments with more than 300 instances establishes the effectiveness of our procedure in relation to approaches previously identified to be best. 相似文献
83.
A gel dosemeter in which ionising radiation causes a colour change was produced by modifying an existing Fricke gel system. This allows a more convenient preparation procedure and gives a better quality dosimetric system for three-dimensional (3-D) dose measurements. The role of three active components of the Ferrous sulphate Xylenol orange Gelatin (FXG) gel dosemeter is quantified with special consideration of their effect on system sensitivity and stability. The optimal composition was found to be 0.5 mM ferrous sulphate, 0.1 mM xylenol orange and 25 mM sulphuric acid. The dose response is linear in the range 0.1–30 Gy. The FXG sensitivity, derived from the gradient of the dose response curve, was found to be ΔA=0.084 cm−1 Gy−1, where A is the optical absorption coefficient at a wavelength of 585 nm, with reproducibility and 24 h stability of better than 5%. 相似文献
84.
R. F. Payne S. P. LaMont R. H. Filby S. E. Glover 《Journal of Radioanalytical and Nuclear Chemistry》2001,248(2):449-452
The parameters for a sulfate based electrodeposition method were optimized for the preparation of Cm and Np alpha-spectrometry sources. Alpha-spectrometry requires the preparation of essentially massless sources to eliminate self-absorption of alpha-particles, which can cause degraded alpha-spectra. A variety of methods for the electrodeposition of actinides have been reported in the literature, many of which require long deposition times and lack reproducibility. A previously reported sulfate based method has been evaluated for the preparation of Np and Cm sources. High yields were achieved and source preparation took 90 minutes or less. The effects of electrodeposition time and pH of the depositing solution were evaluated for each element. Typical resolution (FWHM) for sources prepared by this method is 50 keV or less with recoveries approaching 100%. 相似文献
85.
Amir Lashgari Caroline K. Williams Jenna L. Glover Yueshen Wu Dr. Jingchao Chai Prof. Jianbing “Jimmy” Jiang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(70):16774-16781
The control of the second coordination sphere in a coordination complex plays an important role in improving catalytic efficiency. Herein, we report a zinc porphyrin complex ZnPor8T with multiple flexible triazole units comprising the second coordination sphere, as an electrocatalyst for the highly selective electrochemical reduction of carbon dioxide (CO2) to carbon monoxide (CO). This electrocatalyst converted CO2 to CO with a Faradaic efficiency of 99 % and a current density of −6.2 mA cm−2 at −2.4 V vs. Fc/Fc+ in N,N-dimethylformamide using water as the proton source. Structure-function relationship studies were carried out on ZnPor8T analogs containing different numbers of triazole units and distinct triazole geometries; these unveiled that the triazole units function cooperatively to stabilize the CO2-catalyst adduct in order to facilitate intramolecular proton transfer. Our findings demonstrate that incorporating triazole units that function in a cooperative manner is a versatile strategy to enhance the activity of electrocatalytic CO2 conversion. 相似文献
86.
Fred Glover Darwin Klingman Nancy Phillips 《European Journal of Operational Research》1984,17(1):123-124
In this paper an algorithm is presented for determining the K best paths that may contain cycles in a directed network.The basic idea behind the algorithm is quite simple. Once the best path has been determined it is excluded from the network in such a way that no new path is formed and no more paths are excluded. This step leads to an enlarged network where all the paths, but the best one, can be determined. The method is repeated until the desired paths have been computed.The proposed algorithm can be used not only for the classical K shortest paths problem but also for ranking paths under a nonlinear objective function, provided that an algorithm to determine the best path exists.Computational results are presented and comparisons with other approaches for the classical problem are made. 相似文献
87.
We examine a notion of generalized convex set-valued mapping, extending the notions of a convex relation and a convex process. Under general conditions, we establish duality results for composite set-valued mappings and for convex programming problems involving convex set-valued mappings. We also present applications to the study of economic dynamical systems, by obtaining the characteristics of optimal paths generated by convex processes, and to optimization problems of a certain class of positively homogeneous increasing functions. 相似文献
88.
We propose a new class of foundation-penalty (FP) cuts for MIPs that are easy to generate by exploiting routine penalty calculations. Their underlying concept generalizes the lifting process and provides derivations of major classical cuts. (Gomory cuts arise from low level FP cuts by simply ‘plugging in’ standard penalties.) 相似文献
89.
Paul Zoller Howard W. Starkweather Glover A. Jones 《Journal of Polymer Science.Polymer Physics》1986,24(7):1451-1458
We have combined pressure–volume–temperature measurements and high-temperature x-ray diffraction to calculate the heat of fusion of the poly(4-methyl pentene-1) crystal from the Clapeyron equation. We find ΔHf = 14.8 cal/g, only about half as large as several literature values. The new value of the heat of fusion leads to increased degrees of crystallinity, in agreement with the highly crystalline appearance of the x-ray patterns of typical samples, in particular oriented fibers. The new entropy of fusion at constant pressure of 2.46 cal/deg per mole of monomer units is significantly lower than the values for polypropylene, polybutene-1, and polypentene-1, indicating possible ordering in the melt of this polymer. 相似文献
90.
Consider a finite setE, a weight functionw:E→R, and two matroidsM
1 andM
2 defined onE. The weighted matroid intersection problem consists of finding a setI⊆E, independent in both matroids, that maximizes Σ{w(e):e inI}. We present an algorithm of complexity O(nr(r+c+logn)) for this problem, wheren=|E|,r=min(rank(M
1), rank (M
2)),c=max (c
1,c
2) and, fori=1,2,c
i
is the complexity of finding the circuit ofI∪{e} inM
i
(or show that none exists) wheree is inE andI⊆E is independent inM
1 andM
2. A related problem is to find a maximum weight set, independent in both matroids, and of given cardinalityk (if one exists). Our algorithm also solves this problem. In addition, we present a second algorithm that, given a feasible
solution of cardinalityk, finds an optimal one of the same cardinality. A sensitivity analysis on the weights is easy to perform using this approach.
Our two algorithms are related to existing algorithms. In fact, our framework provides new simple proofs of their validity.
Other contributions of this paper are the existence of nonnegative reduced weights (Theorem 6), allowing the improved complexity
bound, and the introduction of artificial elements, allowing an improved start and flexibility in the implementation of the
algorithms.
This research was supported in part by NSF grant ECS 8503192 to Carnegie-Mellon University. 相似文献