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111.
Zuoying Wen Xiaofeng Tang Chengcheng Wang Christa Fittschen Tao Wang Cuihong Zhang Jiuzhong Yang Yang Pan Fuyi Liu Weijun Zhang 《国际化学动力学杂志》2019,51(3):178-188
Photoionization mass spectrometry as a powerful analytical method has been widely utilized and provided valuable insight in the field of gas-phase reactions. Here, a highly sensitive vacuum ultraviolet (VUV) photoionization time-of-flight mass spectrometer combined with a microwave discharge generator and a fast flow tube reactor has been developed to study radical reactions of atmospheric and combustion interests. Two kinds of continuous light sources, the tunable VUV synchrotron radiation at Hefei, China for isomer-specific product detection and a commercial krypton discharge lamp for time-consuming kinetic measurements, are employed as photoionization sources in the apparatus. A multiplexed detection with high sensitivity (the limit of detection ∼0.8 ppb) and high mass resolution (M/ΔM ∼ 2100) has been approached. As representative examples, the self-reaction of the methyl radical, CH3, and the reaction of the methyl radical with molecular oxygen are studied and multiple species including reactive radicals and isomeric/isobaric products are detected and identified. In addition, some preliminary results related to the reaction kinetics are also presented. 相似文献
112.
Yang Xie Lan-lan Cao Qiang Zhang Jun Chen Gen-bai Chu Yu-jie Zhao Xiao-bin Shan Fu-yi Liu Liu-si Sheng 《化学物理学报(中文版)》2012,25(4):379-388
Vacuum ultraviolet photon-induced ionization and dissociation of isoleucine are investi-gated with synchrotron radiation photoionization mass spectroscopy and theoretical cal-culations. The main fragment ions at m/z=86, 75, 74, 69, 57, 46, 45, 44, 41, 30, 28, and 18 from isoleucine are observed in the mass spectrum at the photon energy of 13 eV. From the photoionization e±ciency curves, appearance energies for the principal fragment ions C5H12N+ (m/z=86)、C2H5NO4+ (m/z=75)、C5H9+ (m/z=69)、C4H9+(m/z=57), and CH4N+(m/z=30) are determined to be 8.84±0.07, 9.25±0.06, 10.20±0.12, 9.25±0.10, and 11.05±0.07 eV, respectively, and possible formation pathways are established in detail by the calculations at the B3LYP/6-31++G(d, p) levels. These proposed channels include simple bond cleavage reactions as well as reactions involving intermediates and transition structures. The experimental and computational appearance energies or barriers are in good agreement. 相似文献
113.
S. Kar Y. K. Ho 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2009,53(3):303-307
We have obtained very accurate excitation energies for helium corresponding to the transitions 2p2
3Pe ↦nln’l’ 3Do
using highly correlated Hylleraas-type wave functions. The doubly excited 2p2
3Pe metastable bound state energy is obtained using Ritz variational principle. The upper bound of 2p2
3Pe energy is –0.7105001556783 a.u., which is close to the best results –0.71050015567833 [R. Hilger et al., Chem. Phys. Lett.
262, 400 (1996)]. We employ complex-coordinate rotation method to obtain 3Do resonances. The 3Do resonance energies and widths along with one-photon two-electron transition energies are reported. 相似文献
114.
D. G. Arbó K. T?kési J. E. Miraglia 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2009,51(3):303-312
We present a theoretical study of the ionization of hydrogen atoms as a result of the interaction with an ultrashort external electric field. Doubly-differential momentum distributions and angular momentum distributions of ejected electrons calculated in the framework of the Coulomb-Volkov and strong field approximations, as well as classical calculations are compared with the exact solution of the time dependent Schr ödinger equation. We show that in the impulsive limit, the Coulomb-Volkov distorted wave theory reproduces the exact solution. The validity of the strong field approximation is probed both classically and quantum mechanically. We found that classical mechanics describes the proper quantum momentum distributions of the ejected electrons right after a sudden momentum transfer, however pronounced the differences at latter stages that arise during the subsequent electron-nucleus interaction. Although the classical calculations reproduce the quantum momentum distributions, it fails to describe properly the angular momentum distributions, even in the limit of strong fields. The origin of this failure can be attributed to the difference between quantum and classical initial spatial distributions. 相似文献
115.
Future perspectives of radiation chemistry are discussed by the analysis of the related information in detail as obtained from our recent surveys of publications and scientific meetings in radiation chemistry and its neighboring research fields, giving some examples, and are summarized as follows. (1) Traditionally important core-parts of radiation chemistry should be activated more. The corresponding research programs are listed in detail. (2) Research fields of physics, chemistry, biology, medicine, and technology in radiation research should interact more among them with each other. (3) Basic research of radiation chemistry should interact more with its applied research. (4) Interface research fields with radiation chemistry should be produced more with mutually common viewpoints and research interests between the two. Interfaces are not only applied research but also basic one. 相似文献
116.
A new approach to determination of the recombination rate of radical ion pairs in moderately polar solvents is presented. It is based on an investigation of transient photocurrents caused by dissociation of exciplexes generated in photoinduced electron transfer reactions. It has been shown that the recombination rate of geminate ion pairs can be found from the photocurrent rise time. We have applied such an approach to transient photocurrents observed by Hirata et al. [Y. Hirata, Y. Kanda, N. Mataga, J. Phys. Chem. 87 (1983) 1659] for the pyrene/dicyanobenzene system in solvents of moderate polarity. The increase of the obtained recombination rate of photogenerated ions with increasing polarity of solvent testifies that ions recombine mainly by the backward electron transfer from the dicyanobenzene anions to solvent-separated cations of pyrene. 相似文献
117.
Dissociative Photoionization of Heterocyclic Molecule-Morpholine under VUV Synchrotron Radiation 下载免费PDF全文
The radiation damage of biomolecules, in particular with aliphatic compound, has been extensively studied. Morpholine is a typical six-membered aliphatic heterocyclic compound. In the present work, photoionization and dissociation of the morpholine monomer and subsequent fragmentations have been investigated by synchrotron vacuum ultraviolet photoionization mass spectrometry and theoretical calculations. The vertical ionization energy of morpholine monomer is 8.37±0.05 eV, which agrees reasonably well with a theoretical value 8.41 eV of morpholine. Experimentally observed fragmentation of morpholine (m/z=87 amu) gives rise to m/z=86 amu, m/z=57 amu, and m/z=29 amu. Based on experimental and theoretical results, it is found that the m/z=86 amu is produced by losingH atom, the m/z=57 amu is formed by the elimination of CH2O with a ring-opening process, the m/z=29 amu is generated by further dissociation of the fragment m/z=57 amu (C3H7N)+ by the elimination of C2H4. This finding would provide valuable insight into the photo-damage of aliphatic compounds, which may be related to living cells and other biological system. 相似文献
118.
We show that the theoretical predictions on high energy behavior of the photoionization cross section of fullerenes depend crucially on the form of the function which approximates the fullerene field. The shape of the high energy cross section is obtained without solving the wave equation. The cross section energy dependence is determined by the analytical properties of the function . 相似文献
119.
Within the effective-mass approximation, we have investigated the binding energies of donor impurities as a function of the wire dimensions and the photoionization cross-section for a hydrogenic donor impurity placed on the center of the quantum well-wire as a function of the normalized photon energy in the GaAs, Ge and Si quantum wires with infinite barriers. The calculations are performed by the variational method based on a two-parametric trial wave function. The results show that the impurity binding energy and the photoionization cross-section depend strongly on both wire dimensions and material parameters. 相似文献
120.
实验研究了钛原子在293~321 nm波段的共振增强多光子电离. 采用激光烧蚀和超声射流相结合的实验技术来制备自由原子,由飞行时间质谱仪实现对钛原子光电离产物的检测. 从离子信号强度对和激光强度的依赖关系导出了钛原子价电子激发态的光电离截面. 实验测量的一些激发态光电离截面在0.2~6.0 Mb. 通过对46Ti、47Ti、48Ti的光电离截面测量研究,没有发现明显的同位素依赖性. 相似文献