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31.
Barrow NS Yates JR Feller SA Holland D Ashbrook SE Hodgkinson P Brown SP 《Physical chemistry chemical physics : PCCP》2011,13(13):5778-5789
Magic-angle spinning (MAS) NMR spin-echo dephasing is systematically investigated for the spin I = 3/2 (11)B nucleus in lithium diborate, Li(2)O·2B(2)O(3). A clear dependence on the quadrupolar frequency (ω(Q)(PAS)/2π = 3C(Q)/[4I(2I- 1)]) is observed: the B3 (larger C(Q)) site dephases more slowly than the B4 site at all investigated MAS frequencies (5 to 20 kHz) at 14.1 T. Increasing the MAS frequency leads to markedly slower dephasing for the B3 site, while there is a much less evident effect for the B4 site. Considering samples at 5, 25, 80 (natural abundance) and 100% (11)B isotopic abundance, dephasing becomes faster for both sites as the (11)B isotopic abundance increases. The experimental behaviour is rationalised using density matrix simulations for two and three dipolar-coupled (11)B nuclei. The experimentally observed slower dephasing for the larger C(Q) (B3) site is reproduced in all simulations and is explained by the reintroduction of the dipolar coupling by the so-called "spontaneous quadrupolar-driven recoupling mechanism" having a different dependence on the MAS frequency for different quadrupolar frequencies. Specifically, isolated spin-pair simulations show that the spontaneous quadrupolar-driven recoupling mechanism is most efficient when the quadrupolar frequency is equal to twice the MAS frequency. While for isolated spin-pair simulations, increasing the MAS frequency leads to faster dephasing, agreement with experiment is observed for three-spin simulations which additionally include the homogeneous nature of the homonuclear dipolar coupling network. First-principles calculations, using the GIPAW approach, of the (2)J(11B-11B) couplings in lithium diborate, metaborate and triborate are presented: a clear trend is revealed whereby the (2)J(11B-11B) couplings increase with increasing B-O-B bond angle and B-B distance. However, the calculated (2)J(11B-11B) couplings are small (0.95, 1.20 and 2.65 Hz in lithium diborate), thus explaining why no zero crossing due to J modulation is observed experimentally, even for the sample at 25% (11)B where significant spin-echo intensity remains out to durations of ~200 ms. 相似文献
32.
Shim JU Patil SN Hodgkinson JT Bowden SD Spring DR Welch M Huck WT Hollfelder F Abell C 《Lab on a chip》2011,11(6):1132-1137
A microfluidic device capable of exploiting the permeability of small molecules through polydimethylsiloxane (PDMS) has been fabricated in order to control the contents of microdroplets stored in storage wells. We demonstrate that protein precipitation and crystallization can be triggered by delivery of ethanol from a reservoir channel, thus controlling the protein solubility in microdroplets. Likewise quorum sensing in bacteria was triggered by delivery of the auto-inducer N-(3-oxododecanoyl)-l-homoserine lactone (OdDHL) through the PDMS membrane of the device. 相似文献
33.
D. Masiyano J. Hodgkinson S. Schilt R. P. Tatam 《Applied physics. B, Lasers and optics》2009,96(4):863-874
We report the effects of self-mixing interference on gas detection using tunable diode laser spectroscopy. For very weak feedback,
the laser diode output intensity gains a sinusoidal modulation analogous to that caused by low finesse etalons in the optical
path. Our experiments show that self-mixing interference can arise from both specular reflections (e.g. cell windows) and
diffuse reflections (e.g. Spectralon™ and retroreflective tape), potentially in a wider range of circumstances than etalon-induced interference. The form and magnitude
of the modulation is shown to agree with theory. We have quantified the effect of these spurious signals on methane detection
using wavelength modulation spectroscopy and discuss the implications for real gas detectors. 相似文献
34.
The theoretical basis behind a recent quantitative analysis of 17O exchange in ZrW2O8 [M.R. Hampson, J.S.O. Evans, P. Hodgkinson, J. Am. Chem. Soc. 127 (2005) 15175-15181] is set out. Despite the complexities of combining the multi-exponential relaxation of half-integer quadrupolar nuclei with chemical exchange, it is shown how magnetisation transfer experiments can be analysed to obtain estimates of absolute exchange rates. The multi-exponential relaxation is best modelled using a magnetic mechanism, i.e. the rapid T1 relaxation observed, particularly at high temperatures, can be directly related to the relatively high degree of 17O labelling employed. The combination of the 1D EXSY results with T1 values as a function of temperature provides exchange rates and activation barriers over a wide temperature range (40-226 degrees C). 相似文献
35.
36.
F. Mackenzie T. G. Hodgkinson S. A. Cassidy P. Healey 《Optical and Quantum Electronics》1992,24(4):S491-S504
A technology which may form a powerful optical interconnection scheme based on a bus architecture is presented. It is shown that the fibre array connectors involved require alignment tolerances comparable to those of present electrical connectors. Further system flexibility can be obtained by tailoring the connector wavelength characteristics. Results of an experiment, where distributed amplification within the backplane of an optical bus was used to compensate for the power removed at the access points, are also presented. This allows a significantly higher number of output ports to be served than would be possible using a passive bus. As an example application, the feasibility of using the technology as the backplane interconnection in a card and rack system is demonstrated. Extension to a switching scheme using the multi-dimensional optical network concept is described. 相似文献
37.
The excitation of an N-level quantum oscillator by a strong oscillating electric field in the presence of external perturbations can in general be described by a Boltzmann equation for the density matrix. In this paper it is shown that under certain circumstances this may be reduced to a set of rate equations for the level populations. In contrast to the weak field situation, these rate equations explicitly contain multi-photon transition rates. 相似文献
38.
39.
Gobetto R Nervi C Chierotti MR Braga D Maini L Grepioni F Harris RK Hodgkinson P 《Chemistry (Weinheim an der Bergstrasse, Germany)》2005,11(24):7461-7471
Fumaric, malonic, maleic, and hydromuconic (HOOCCH2(CH)2CH2COOH) acids were used to prepare a series of hydrogen-bonded adducts or salts, depending on whether acid-base proton transfer takes place, with the dibase [N(muCH2CH2)3N] in various stoichiometric ratios. The resulting compounds have been investigated by using the 1H MAS, 15N, and 13C cross polarisation magic-angle spinning (CPMAS) methods and discussed in relation to X-ray diffraction studies to ascertain the nature of the O-HO, NH-O, and N+-HO- hydrogen bonds between the various species. In addition, two polymorphic forms of the malonic compound and a hydrate in the maleic case were examined. We also present the correlations between the chemical shifts of the hydrogen-bonded protons and those from the proton transfer reaction (acid-to-base) with the heavy atom distances. The dynamic behaviour in the solid-state of the [N(muCH2CH2)3N] adducts with fumaric 2:1, maleic 1:1 hydrate, and hydromuconic acids, and a malonate 2:1 polymorph adduct have been investigated by using variable-temperature 1H spin-lattice relaxation times. A substantial agreement between the activation energies obtained from fitting the T1 data and the results of potential energy barrier calculations demonstrates that the facile reorientation of the [N(muCH2CH2)3N] molecule occurs in several of the adducts. 相似文献
40.
This paper addresses the use of different slotted pores in rotating membrane emulsification technology.Pores of square and rectangular shapes were studied to understand the effect of aspect ratio (1-3.5) and their orientation on oil droplet formation.Increasing the membrane rotation speed decreased the droplet size,and the oil droplets produced were more uniform using slotted pores as compared to circular geometry.At a given rotation speed,the droplet size was mainly determined by the pore size and the fluid velocity of oil through the pore (pore fluid velocity).The ratio of droplet diameter to the equivalent diameter of the slotted pore increased with the pore fluid velocity.At a given pore fluid velocity and rotation speed,pore orientation significantly influences the droplet formation rate: horizontally disposed pores (with their longer side perpendicular to the membrane axis) generate droplets at double the rate of vertically disposed pores.This work indicates practical benefits in the use of slotted membranes over conventional methods. 相似文献