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91.
92.
Zhan Yu Lee Chuin Chen Rosa Erra‐Balsells Hiroshi Nonami Kenzo Hiraoka 《Rapid communications in mass spectrometry : RCM》2010,24(11):1507-1513
Probe electrospray ionization (PESI) is a modified version of the electrospray ionization (ESI), where the capillary for sampling and spraying is replaced by a solid needle. High tolerance to salts and direct ambient sampling are major advantages of PESI compared with conventional ESI. In this study, PESI‐MS was used to monitor some biological and chemical reactions in real‐time, such as acid‐induced protein denaturation, hydrogen/deuterium exchange (HDX) of peptides, and Schiff base formation. By using PESI‐MS, time‐resolved mass spectra and ion chromatograms can be obtained reproducibly. Real‐time PESI‐MS monitoring can give direct and detailed information on each chemical species taking part in reactions, and this is valuable for a better understanding of the whole reaction process and for the optimization of reaction parameters. PESI‐MS can be considered as a potential tool for real‐time reaction monitoring due to its simplicity in instrumental setup, direct sampling with minimum sample preparation and low sample consumption. Copyright © 2010 John Wiley & Sons, Ltd. 相似文献
93.
Lau Cher Hon Cervini Raoul Clarke Stephen R. Markovic Milena Ginic Matisons Janis G. Hawkins Stephen C. Huynh Chi P. Simon George P. 《Journal of nanoparticle research》2008,10(1):77-85
Nanosized powders of Ti-Nb oxide core-shell nanocrystals with atomic ratios of Nb/Ti = 0.11, 0.25, and 0.38 have been prepared
by two preparation routes. The first route was co-precipitation, followed by␣annealing, using NbCl5 as a source of Nb. The second route was coating of pure TiO2 nanocrystals by Nb-isopropoxide in liquid medium, followed by impregnation of the Nb into the nanoparticles by annealing.
Both methods yielded anatase nanocrystals with a Nb-rich shell and a core, which had much lower Nb loadings. The anatase structure
solid solution (with Nb incorporated) was stable under annealing up to 760°C. The particle size remained within the nanometric
scale (<50 nm) under heat-treatment up to 760°C. It has been shown that the fabricated powders can be redispersed in aqueous media
by simple ultrasound treatment, resulting in nanosized dispersions. Using a variety of analytical techniques, including depth
profiling of single nanocrystallites by AES combined with sputtering by Ar ions, the mechanism of the core-shell structure
creation was studied. It is proposed that the formation of the core-shell structure is governed by solubility limitations
in the co-precipitation route and by solubility and diffusion limitations in the coating-incorporation route. 相似文献
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96.
Photoelectron energy distribution curves from solid CO2 have been determined for excitation energies from hv = 14 up to 40 eV using synchrotron radiation. A 1:1 correspondence to the gas-phase photoelectron spectrum is observed for the occupied molecular orbitals. The vertical binding energies EBv (EVAC = 0) and widths (fwhm) of the valence bands of solid CO2 are determined to be 13.0 and 0.95 eV (1πg); 16.7 and 1.1 eV (1πu); 17.6 and 0.85 eV (3σu) and 18.8 and 0.8 eV (4σg) for the individual bands respectively. The partial photoemission cross sections differ importantly from those of the gas phase in exhibiting pronounced maxima at 5.2 eV (1πg), 4.4–5.3 eV (1πu + 3σu) and 4.2 eV (4σg) above the vacuum level, which is attributed to effects of high density of final (conduction-band) states. Further weaker maxima are observed at higher photon energies. Contrary to the case for the gas phase, the resonances are unperturbed in the solid by degenerate autoionizing molecular Rydberg states. The molecular origin of the resonances in the continuum is discussed and related to X-ray absorption spectra, electron-scattering data and to theoretical cross-section calculations. It is shown that the same set of resonances is observed in the different experiments. The resonances occur however at different energies due to different Coulomb interactions. The photoemission results presented provide also a key to the hitherto unexplained optical spectrum of solid CO2 in the VUV range, making possible an assignment of the structures observed to Frenkel-type excitons (hv ≤ 15 eV) and interband transitions (hv ? 15 eV). 相似文献
97.
Coherent anti-Stokes Raman scattering (CARS) spectra of excited molecules as well as Shpolskii spectra provide information about geometry changes between ground and excited states. Vibrational frequencies and relative intensities from recently obtained CARS spectra of the chrysene S1 and T1 state and earlier observed Shpolskii spectra are interpreted in terms of molecular geometry and force-field changes by means of quantum-chemical consistent force field (QCFF) and Franck-Condon factor calculations. The comparison of observed and calculated relative intensities indicates a coupling between the S1 and S2 state enhancing some of the vibrational radiative singlet transitions both in absorption and fluorescence spectra whereas within the phosphorescence spectra proportionality to calculated Franck-Condon factors is obeyed. The T1 state is the more loosely bound state and its geometry change is different from that of the S1 state. The resonance CARS transitions in the S1 state are assigned to totally symmetric vibrations getting their intensity by a coupling scheme analogous to the A term of the resonance Raman effect: the relative intensity of a transition is shown to be proportional to the Franck-Condon factor to the higher excited state and to the squared vibrational frequency. Using this relation this state can be identified by means of its finger-print-like intensity pattern. 相似文献
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99.
For a gaussian broadband radiation field (multimode laser without phase-correlation) the bleaching behaviour of a homogeneously broadened two level system is investigated in dependence on the spectral width (δυ) of the field. Taking into consideration the coherent mode-interaction, originating from the nonstationary reaction of population inversion on the fluctuations of the radiation field, a decrease of the bleaching effect results as soon as the spectral width δυ becomes larger than ⊥1 = 1/T1 with T1 the longitudinal relaxation time of the molecular transition concerned. Neglecting this effect in the analysis of broadband bleaching measurements can result in the unjustified assumption of an inhomogeneous broadening of the spectral band under consideration, which has consequences on the magnitude of the molecular absorption cross-section derived from these measurements. 相似文献
100.
We present a novel, simple asymptotic expansion for the spectrum of radiation that is backscattered from a laser by a counterpropagating (or copropagating) electron. The solutions are presented in such a way that they explicitly show the relative merit of using an intense laser and of an energetic electron beam in x-ray production in the single particle regime. Simple scaling laws are given. 相似文献