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61.
62.
Gamsey S Miller A Olmstead MM Beavers CM Hirayama LC Pradhan S Wessling RA Singaram B 《Journal of the American Chemical Society》2007,129(5):1278-1286
Several novel diboronic acid-substituted bipyridinium salts were prepared and, using a fluorescent reporter dye, were tested for their ability to selectively bind various monosaccharides and alpha-hydroxycarboxylates in an aqueous medium. The fluorescence sensing mechanism relies on the formation of a ground-state charge-transfer complex between the dye and bipyridinium. An X-ray crystal structure of this complex is described herein. Glucose selectivity over fructose and galactose was achieved by designing the bipyridinium-based receptors to be capable of attaining a 1:1 receptor/substrate stoichiometry via cooperative diboronic acid binding. 相似文献
63.
Stone N Hart Prieto MC Crow P Uff J Ritchie AW 《Analytical and bioanalytical chemistry》2007,387(5):1657-1668
Near-infrared Raman spectroscopy, an optical technique that is able to interrogate biological tissues, has been used to study
bladder and prostate tissues, with the objective being to provide a first approximation of gross biochemical changes associated
with the process of carcinogenesis. Prostate samples for this study were obtained by taking a chip at TURP, and bladder samples
from a biopsy taken at TURBT and TURP, following ethical approval. Spectra were taken from purchased biochemical constituents
and different pathologies within the bladder and the prostate. We were then able to determine the biochemical basis for these
pathologies by utilising an ordinary least-squares fit. We have shown for the first time that we are able to utilise Raman
spectroscopy in determining the biochemical basis for the different pathologies within the bladder and prostate gland. In
this way we can achieve a better understanding of disease processes such as carcinogenesis. This could have major implications
in the future of the diagnosis of disease within the bladder and the prostate gland. 相似文献
64.
The translational anisotropy and rotational angular momentum polarization of a selection of rotational states of the O2 (a 1Deltag; v=0) photofragment formed from ozone photolysis at 248, 260, and 265 nm have been determined using the technique of resonance enhanced multiphoton ionization in combination with time of flight mass spectrometry. At 248 nm, the dissociation is well described as impulsive in nature with all rotational states exhibiting similarly large, near-limiting values for the bipolar moments describing their angular momentum alignment and orientation. At 265 nm, however, the angular momentum polarization parameters determined for consecutive odd and even rotational states exhibit clear differences. Studies at the intermediate wavelength of 260 nm strongly suggest that such a difference in the angular momentum polarization is speed dependent and this proposal is consistent with the angular momentum polarization parameters extracted and reported previously for longer photolysis wavelengths [G. Hancock et al., Phys. Chem. Chem. Phys. 5, 5386 (2003); S. J. Horrocks et al., J. Chem. Phys. 126, 044308 (2007)]. The alternation of angular momentum polarization for successive odd and even J states may be a consequence of the different mechanisms leading to the formation of the two O2 (a 1Deltag) Lambda doublets. Specifically, the involvement of out of plane parent rotational motion is proposed as the origin for the observed depolarization for the Delta- relative to the Delta+ state. 相似文献
65.
A procedure that rapidly generates an approximate parametric representation of macromolecular surface shapes is described. The parametrization is expressed as an expansion of real spherical harmonic basis functions. The advantage of using a parametric representation is that a pair of surfaces can be matched by using a quasi-Newton algorithm to minimize a suitably chosen objective function. Spherical harmonics are a natural and convenient choice of basis function when the task is one of search in a rotational search space. In particular, rotations of a molecular surface can be simulated by rotating only the harmonic expansion coefficients. This rotational property is applied for the first time to the 3-dimensional molecular similarity problem in which a pair of similar macromolecular surfaces are to be maximally superposed. The method is demonstrated with the superposition of antibody heavy chain variable domains. Special attention is given to computational efficiency. The spherical harmonic expansion coefficients are determined using fast surface sampling and integration schemes based on the tessellation of a regular icosahedron. Low resolution surfaces can be generated and displayed in under 10 s and a pair of surfaces can be maximally superposed in under 3 s on a contemporary workstation. ©1999 John Wiley & Sons, Inc. J Comput Chem 20: 383–395, 1999 相似文献
66.
Gamsey S Suri JT Wessling RA Singaram B 《Langmuir : the ACS journal of surfaces and colloids》2006,22(21):9067-9074
A fluorescent anionic dye and a viologen appended with boronic acids, which serve as glucose receptors, have been synthesized and immobilized into a poly(2-hydroxyethyl methacrylate) hydrogel for use as a continuous glucose monitor. The fluorescence of the dye is modulated by the quenching efficiency of the viologen-based receptor, which in turn is dependent on the glucose concentration. Two monomeric versions of the quencher/receptor unit were prepared and their performance within the hydrogel evaluated. By tethering the quencher/receptor to the hydrogel matrix using a single-point attachment, slightly improved glucose sensing was observed. The hydrogels were tested for their ability to continuously and reversibly detect glucose over the course of several hours. The tests were carried out using a cuvette-based system, as well as a fiber-optic-based configuration. Under physiological conditions (0.1 M phosphate buffer, pH 7.4, 37 degrees C), the fluorescent hydrogels display an excellent dynamic response to glucose concentrations within the biologically significant range (2.5-20 mM). 相似文献
67.
Matthew R. Begley Noah R. Philips Brett G. Compton David V. Wilbrink Robert O. Ritchie Marcel Utz 《Journal of the mechanics and physics of solids》2012,60(8):1545-1560
This paper describes a micromechanical analysis of the uniaxial response of composites comprising elastic platelets (bricks) bonded together with thin elastic perfectly plastic layers (mortar). The model yields closed-form results for the spatial variation of displacements in the bricks as a function of constituent properties, which can be used to calculate the effective properties of the composite, including elastic modulus, strength and work-to-failure. Regime maps are presented which indicate critical stresses for failure of the bricks and mortar as a function of constituent properties and brick architecture. The solution illustrates trade-offs between elastic modulus, strength and dissipated work that are a result of transitions between various failure mechanisms associated with brick rupture and rupture of the interfaces. Detailed scaling relationships are presented with the goal of providing material developers with a straightforward means to identify synthesis targets that balance competing mechanical behaviors and optimize material response. Ashby maps are presented to compare potential brick and mortar composites with existing materials, and identify future directions for material development. 相似文献
68.
K. E. Whittaker L. Ciaffoni G. Hancock P. L. Hurst R. Peverall G. A. D. Ritchie 《Applied physics. B, Lasers and optics》2014,116(1):157-168
Studies into the suitability of a novel, widely tunable telecom L-band (1,563–1,613 nm) digital supermode distributed Bragg reflector (DS-DBR) laser for cavity ring-down spectroscopy (CRDS) are presented. The spectrometer comprised of a 36.6?cm long linear cavity with ring-down times varying between 19–26 μs across the 50 nm DS-DBR wavelength range due to changes in the cavity mirror reflectivities with wavelength. The potential of such a broadband, high-resolution CRD spectrometer was illustrated by investigating several transitions of CO2 in air, a 5 % calibrated mixture and breath samples. Allan variance measurements at a single wavelength indicated an optimal minimum detectable absorption coefficient (α min) of 3 × 10?10 cm?1 over 20 s. 相似文献
69.
Ritchie MA Gill AC Deery MJ Lilley K 《Journal of the American Society for Mass Spectrometry》2002,13(9):1065-1077
The structure of N-linked glycans is determined by a complex, anabolic, intracellular pathway but the exact role of individual glycans is not always clear. Characterization of carbohydrates attached to glycoproteins is essential to aid understanding of this complex area of biology. Specific mass spectral detection of glycopeptides from protein digests may be achieved by on-line HPLC-MS, with selected ion monitoring (SIM) for diagnostic product ions generated by cone voltage fragmentation, or by precursor ion scanning for terminal saccharide product ions, which can yield the same information more rapidly. When glycosylation is heterogeneous, however, these approaches can result in spectra that are complex and poorly resolved. We have developed methodology, based around precursor ion scanning for ions of high m/z, that allows site specific detection and structural characterization of glycans at high sensitivity and resolution. These methods have been developed using the standard glycoprotein, fetuin, and subsequently applied to the analysis of the N-linked glycans attached to the scrapie-associated prion protein, PrP(Sc). These glycans are highly heterogeneous and over 30 structures have been identified and characterized site specifically. Product ion spectra have been obtained on many glycopeptides confirming structure assignments. The glycans are highly fucosylated and carry Lewis X or sialyl Lewis X epitopes and the structures are in-line with previous results. 相似文献
70.
We study the magnetotransport of a GaAs/AlGaAs quantum well with self-assembled InAs quantum dots. Negative magnetoresistance is observed at low field and analysed by weak localization theory. The temperature dependence of the extracted dephasing rate is linear, which shows that the inelastic electron-electron scattering processes with small energy transfer are the dominant contribution in breaking the electron phase coherence. The results are compared with those of a reference sample that contains no quantum dots. 相似文献