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11.
Photocatalytic Water Oxidation by a Pyrochlore Oxide upon Irradiation with Visible Light: Rhodium Substitution Into Yttrium Titanate 下载免费PDF全文
Borbala Kiss Dr. Christophe Didier Timothy Johnson Dr. Troy D. Manning Dr. Matthew S. Dyer Dr. Alexander J. Cowan Dr. John B. Claridge Prof. James R. Darwent Prof. Matthew J. Rosseinsky 《Angewandte Chemie (International ed. in English)》2014,53(52):14480-14484
A stable visible‐light‐driven photocatalyst (λ≥450 nm) for water oxidation is reported. Rhodium substitution into the pyrochlore Y2Ti2O7 is demonstrated by monitoring Vegard′s law evolution of the unit‐cell parameters with changing rhodium content, to a maximum content of 3 % dopant. Substitution renders the solid solutions visible‐light active. The overall rate of oxygen evolution is comparable to WO3 but with superior light‐harvesting and surface‐area‐normalized turnover rates, making Y2Ti1.94Rh0.06O7 an excellent candidate for use in a Z‐scheme water‐splitting system. 相似文献
12.
Kosikov KM Gorin AA Lu XJ Olson WK Manning GS 《Journal of the American Chemical Society》2002,124(17):4838-4847
DNA dodecamers of the alternating d(CG).d(CG) sequence with six phosphate groups either charge-neutralized or substituted by neutral methylphosphonates across the major or minor groove have been subjected to energy minimization to determine the conformational effect of the asymmetric elimination of phosphate charge. We report bending angles, directions of bending, and detailed structural characteristics such as groove widths and local base-pair parameters. Our principal results are that charge neutralization on one face of the DNA induces significant bending toward the neutralized face, in agreement with theoretical predictions on a simplified model and experimental data on a similar base-pair sequence, and that the DNA conformation averaged over all stereospecific methylphosphonate substitutions is nearly the same as the conformation produced by charge neutralization of the phosphates. Individual isomers, however, cover a wide range of structures, with the magnitude and direction of overall bending sensitive to the precise stereochemical pattern of neutralization. Our simulation does not explicitly contain counterions, and the results therefore suggest that counterions can influence DNA structure by neutralizing the phosphate charge. These data provide new hints into the molecular mechanisms which underlie the deformations of DNA structure induced by the binding of positively charged proteins and other tightly associated cationic species. 相似文献
13.
R. Manning 《Optical and Quantum Electronics》1971,3(2):93-97
This paper gives a unified theoretical analysis of Laser Doppler systems covering both the optical and electronic aspects, and applicable to all systems which have either a real or virtual fringe pattern. Previous experimental results by Greated for the Doppler spectrum are confirmed and in addition a fuller treatment of the low frequency part of the spectrum is presented. 相似文献
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15.
Irradiation of zinc selenide at ~ 20°K with electrons capable of displacing zinc atoms results in the production of cathodoluminescence emission bands at 610 and 630 nm. Enhancement of the 630 nm emission band by electron damage requires the presence of copper in the samples. These emissions have been shown to give a peak energy shift to lower energies after excitation, as is characteristic of donor-acceptor pair recombination. It is concluded that the 610 and 630 nm emission bands of zinc selenide are equivalent to the self-activated and copper green emission bands of zinc sulphide. The 530 nm emission band of zinc selenide is not sensitive to electron damage, shows no time shift and is thought to be equivalent to the copper blue emission of zinc sulphide. 相似文献
16.
McGowan RS Nittrouer S Manning CJ 《The Journal of the Acoustical Society of America》2004,115(2):871-884
Beginning at the age of about 14 months, eight children who lived in a rhotic dialect region of the United States were recorded approximately every 2 months interacting with their parents. All were recorded until at least the age of 26 months, and some until the age of 31 months. Acoustic analyses of speech samples indicated that these young children acquired [inverted r] production ability at different ages for [inverted r]'s in different syllable positions. The children, as a group, had started to produce postvocalic and syllabic [inverted r] in an adult-like manner by the end of the recording sessions, but were not yet showing evidence of having acquired prevocalic [inverted r]. Articulatory limitations of young children are posited as a cause for the difference in development of [inverted r] according to syllable position. Specifically, it is speculated that adult-like prevocalic [inverted r] production requires two lingual constrictions: one in the mouth, and the other in the pharynx, while postvocalic and syllabic [inverted r] requires only one oral constriction. Two lingual constrictions could be difficult for young children to produce. 相似文献
17.
Molality as a unit of measure for expressing 1H MRS brain metabolite concentrations in vivo 总被引:1,自引:0,他引:1
Knight-Scott J Haley AP Rossmiller SR Farace E Mai VM Christopher JM Manning CA Simnad VI Siragy HM 《Magnetic resonance imaging》2003,21(7):787-797
Absolute concentrations of cerebral metabolite in in vivo 1H magnetic resonance spectroscopy studies (1H-MRS) are widely reported in molar units as moles per liter of tissue, or in molal units as moles per kilogram of tissue. Such measurements require external referencing or assumptions as to local water content. To reduce the scan time, avoid assumptions that may be invalid under specific pathologies, and provide a universally accessible referencing procedure, we suggest that metabolite concentrations from 1H-MRS measurements in vivo be reported in molal units as moles per kilogram of tissue water. Using internal water referencing, a two-compartment water model, a simulated brain spectrum for peak identification, and a spectroscopic bi-exponential spin-spin relaxation segmentation technique, we measured the absolute concentrations for the four common 1H brain metabolites: choline (Cho), myo-inositol (mIno), phosphocreatine + creatine (Cr), and N-acetyl-aspartate (NAA), in the hippocampal region (n = 26) and along the Sylvian fissure (n = 61) of 35 healthy adults. A stimulated echo localization method (20 ms echo time, 10 ms mixing time, 4 s repetition time) yielded metabolite concentrations, uncorrected for metabolite relaxation or contributions from macromolecule resonances, that were expectantly higher than with molar literature values. Along the Sylvian fissure the average concentrations (coefficient of variation (CV)) in mmoles/kg of tissue water were 17.6 (12%) for NAA, 14.2 (9%) for Cr, 3.6 (13%) for Cho, and 13.2 (15%) for mIno. Respective values for the hippocampal region were 15.7 (20%), 14.7 (16%), 4.6 (19%), and 17.7 (26%). The concentrations of the two regions were significantly different (p = 0.001) for NAA, mIno, and Cho, a trend in agreement with previous studies. All gray matter Sylvian fissure CV values, except for NAA, were also in agreement with previous 1H-MRS gray matter studies. The reduced precision of the NAA concentration was attributed to overlapping signal contributions from glutamate and glutamine (Glx), suggesting that a detailed Glx model is critical for accurate quantitation of the NAA 2.02 ppm resonance. The reduced precision of the measurements in the hippocampal region was attributed to poor spectral resolution. 相似文献
18.
Anthony Manning 《Bulletin of the Brazilian Mathematical Society》1992,22(2):157-177
The trouble with Newton's method for finding the roots of a complex polynomial is knowing where to start the iteration. In this paper we apply the theory of rational maps and some estimates based on distortion theorems for univalent functions to find lower bounds, depending only on the degreed, for the size of regions from which the iteration will certainly converge to a root. We can also bound the number of iterations required and we give a method that works for every polynomial and takes at most some constant timesd
2(logd)2 log(d
3/) iterations to find one root to within an accuracy of . 相似文献
19.
Manning GS 《Journal of the American Chemical Society》2003,125(49):15087-15092
X-ray diffraction structures of the nucleosome core particle along with a variety of experiments are consistent with the idea that an important source of the free energy holding DNA to the superhelical ramp on the histone octamer surface is obtained from a relatively small amount of electrostatic neutralization of the DNA phosphate charge by positively charged histone groups, especially arginine residues. Here we present a theoretical analysis of a simple model that emphasizes the competition between the high degree of bending of the stiff DNA molecule required for its tight curvature on the histone octamer and the neutralization of the DNA phosphate charge by basic histone residues. Our calculation accounts for the strong influence of condensed counterions on the electrostatic interactions. We find that the minimum amount of free energy required to bend DNA into axial conformity with the superhelical ramp at physiological salt concentration can be provided by a scant 6% neutralization of the phosphate charge, in close correspondence to the stoichiometric neutralization of phosphate charge by the arginine side chain that intrudes into the inward-facing minor groove of each DNA double helical turn. 相似文献
20.
Many of the interferences reported earlier for the determination of manganese in a graphite furnace were not found when a modern graphite furnace was used. At high levels of chloride matrix, an interference which was observed in the modern furnace was reduced when manganese was determined under constant temperature conditions. In this work, the sample was introduced on a tungsten wire after the graphite furnace had reached a constant, preset temperature. Drying and ashing were accomplished outside the atomization furnace, reducing contamination from matrix materials. 相似文献