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41.
The recent discovery of the new smectic-C(d6)(*) (SmC(d6)(*)) phase [S. Wang et al., Phys. Rev. Lett. 104, 027801 (2010)] also revealed the existence of a noisy region in the temperature window between the SmC(d6)(*) phase and the smectic-C(d4)(*) (SmC(d4)(*)) phase. Characterized by multiple resonant peaks spanning a wide region in Q(Z), the corresponding structure of this temperature window has been a mystery. In this Letter, through a careful resonant x-ray diffraction study and simulations of the diffraction spectra, we show that this region is in fact an unusually large coexistence region of the SmC(d6)(*) phase and the SmC(d4)(*) phase. The structure of the noisy region is found to be a heterogeneous mixture of local SmC(d6)(*) and SmC(d4)(*) orders on the sub-μm scale. 相似文献
42.
Miller EM Sheps L Lu YJ Case AS McCoy AB Lineberger WC 《The Journal of chemical physics》2012,136(4):044313
Negative-ion photoelectron spectroscopy of ICN(-) (X??(2)Σ(+)) reveals transitions to the ground electronic state (X??(1)Σ(+)) of ICN as well as the first five excited states ((3)Π(2), (3)Π(1), Π(0(-) ) (3), Π(0(+) ) (3), and (1)Π(1)) that make up the ICN A continuum. By starting from the equilibrium geometry of the anion, photoelectron spectroscopy characterizes the electronic structure of ICN at an elongated I-C bond length of 2.65 A?. Because of this bond elongation, the lowest three excited states of ICN ((3)Π(2), (3)Π(1), and Π(0(-) ) (3)) are resolved for the first time in the photoelectron spectrum. In addition, the spectrum has a structured peak that arises from the frequently studied conical intersection between the Π(0(+) ) (3) and (1)Π(1) states. The assignment of the spectrum is aided by MR-SO-CISD calculations of the potential energy surfaces for the anion and neutral ICN electronic states, along with calculations of the vibrational levels supported by these states. Through thermochemical cycles involving spectrally narrow transitions to the excited states of ICN, we determine the electron affinity, EA(ICN), to be 1.34(5) (+0.04∕-0.02) eV and the anion dissociation energy, D(0)(X??(2)Σ(+) I-CN(-)), to be 0.83 (+0.04/-0.02) eV. 相似文献
43.
Gerardi HK DeBlase AF Leavitt CM Su X Jordan KD McCoy AB Johnson MA 《The Journal of chemical physics》2012,136(13):134318
The (HCOOH)(2) anion, formed by electron attachment to the formic acid dimer (FA(2)), is an archetypal system for exploring the mechanics of the electron-induced proton transfer motif that is purported to occur when neutral nucleic acid base-pairs accommodate an excess electron [K. Aflatooni, G. A. Gallup, and P. D. Burrow, J. Phys. Chem. A 102, 6205 (1998); J. H. Hendricks, S. A. Lyapustina, H. L. de Clercq, J. T. Snodgrass, and K. H. Bowen, J. Chem Phys. 104, 7788 (1996); C. Desfrancois, H. Abdoul-Carime, and J. P. Schermann, ibid. 104, 7792 (1996)]. The FA(2) anion and several of its H∕D isotopologues were isolated in the gas phase and characterized using Ar-tagged vibrational predissociation and electron autodetachment spectroscopies. The photoelectron spectrum of the FA(2) anion was also recorded using velocity-map imaging. The resulting spectroscopic information verifies the equilibrium FA(2)(-) geometry predicted by theory which features a symmetrical, double H-bonded bridge effectively linking together constituents that most closely resemble the formate ion and a dihydroxymethyl radical. The spectroscopic signatures of this ion were analyzed with the aid of calculated anharmonic vibrational band patterns. 相似文献
44.
El-Sayed A. El-Sheikh Mahmoud M. Ramadan Ahmed E. El-Sobki Ali A. Shalaby Mark R. McCoy Ibrahim A. Hamed Mohamed-Bassem Ashour Bruce D. Hammock 《Molecules (Basel, Switzerland)》2022,27(22)
The use of pesticides leads to an increase in agricultural production but also causes harmful effects on human health when excessively used. For safe consumption, pesticide residues should be below the maximum residual limits (MRLs). In this study, the residual levels of pesticides in vegetables and fruits collected from farmers’ markets in Sharkia Governorate, Egypt were investigated using LC-MS/MS and GC-MS/MS. A total number of 40 pesticides were detected in the tested vegetable and fruit samples. Insecticides were the highest group in detection frequency with 85% and 69% appearance in vegetables and fruits, respectively. Cucumber and apple samples were found to have the highest number of pesticide residues. The mean residue levels ranged from 7 to 951 µg kg−1 (in vegetable samples) and from 8 to 775 µg kg−1 (in fruit samples). It was found that 35 (40.7%) out of 86 pesticide residues detected in vegetables and 35 (38.9%) out of 90 pesticide residues detected in fruits exceeded MRLs. Results for lambda-cyhalothrin, fipronil, dimothoate, and omethoate in spinach, zucchini, kaki, and strawberry, respectively, can cause acute or chronic risks when consumed at 0.1 and 0.2 kg day−1. Therefore, it is necessary for food safety and security to continuously monitor pesticide residues in fruits and vegetables in markets. 相似文献
45.
James A. McCoy 《Mathematische Zeitschrift》2004,246(1-2):155-166
46.
47.
The vibrations of H3O2- and D3O2- are investigated using diffusion Monte Carlo (DMC) and vibrational configuration-interaction approaches, as implemented in the program MULTIMODE. These studies use the potential surface recently developed by Huang et al. [ J. Am. Chem. Soc. 126, 5042 (2004)]. The focus of this work is on the vibrational ground state and fundamentals which occur between 100 and 3700 cm(-1). In most cases, excellent agreement is obtained between the fundamental frequencies calculated by the two approaches. This serves to demonstrate the power of both methods for treating this very anharmonic system. Based on the results of the MULTIMODE and DMC treatments, the extent and nature of the couplings in H3O2- and D3O2- are investigated. 相似文献
48.
Distribution kinetics of Ostwald ripening at large volume fraction and with coalescence 总被引:1,自引:0,他引:1
Condensation phase transitions from metastable fluids occur by nucleation with accompanying particle growth and eventual Ostwald ripening. During ripening the subcritical particles dissolve spontaneously while larger particles grow and possibly coalesce if their volume fraction is large enough. The classical diffusion-influenced rates are also affected by large particle concentrations and are here described by mass-dependent rates. We represent the kinetics of ripening through growth, dissolution, and biparticle coalescence by a new population dynamics equation for the particle size distribution (PSD). Numerical solutions of the scaled governing equations show that coalescence plays a major role in influencing the PSD when the scaled mass concentration (volume fraction) or number concentration is relatively large. The solution describes the time range from initial conditions to the final narrowing of polydispersity. We show that the time dependence of the average particle mass in the asymptotic period of ripening has a power-law increase dependent on rate expressions for particle growth and coalescence at large values of volume fraction. 相似文献
49.
Gelation can occur in polymer, hydrogel, and colloid systems that undergo reversible aggregation-fragmentation (crosslinking accompanied by breakage). Gelation, characterized by rapid divergence of weight-average molecular weight and viscosity due to initial network formation, can be reversed if conditions change. In this paper, reversible aggregation and fragmentation in the pre-gelation time period are modeled with distribution kinetics. Moment equations are obtained from the population balance equation, and solved for eight different rate kernels. We identify the cases for which gelation is possible and obtain the critical values for the rate constants that allow gelation. The model provides a good simulation of published experimental data for aggregation and degradation of plasticized wheat gluten during thermo-mechanical treatments. We also evaluate two closure approximations based on Gamma and log-normal distributions, and conclude that log-normal closure predicts all five possible steady states, in agreement with the Vigil-Ziff criterion, and Gamma closure predicts only three. However, Gamma closure approximates the steady state either closely or exactly, whereas log-normal closure only poorly approximates the steady-state distribution. 相似文献
50.
McCoy LF Scholl PF Schleicher RL Groopman JD Powers CD Pfeiffer CM 《Rapid communications in mass spectrometry : RCM》2005,19(16):2203-2210
A method for quantitative analysis of aflatoxin B1-lysine adduct (B1-Lys) in serum by liquid chromatography using tandem mass spectrometry (LC/MS/MS) is presented. The protein in a 250-microL sample was digested in the presence of a stable-isotope internal standard during a 4-h incubation at 37 degrees C with Pronasetrade mark. B1-Lys and the internal standard were extracted using mixed-mode solid-phase extraction cartridges and eluted with 2% formic acid in methanol. Following evaporation and reconstitution, extracts were injected onto a Luna C-18(2) column and eluted with a step gradient of acetonitrile and 0.06% formic acid. The B1-Lys and the internal standard were detected in a positive ionization selective reaction monitoring mode with a ThermoFinnigan TSQ Quantum triple quadrupole mass spectrometer. Calibration curves were linear for concentrations from 0.05-8.0 ng/mL. The method was validated with aflatoxin B1 dosed rat serum diluted to anticipated high and low concentrations. Total imprecision determined from 30 measurements over 15 days was 5.6% and 9.1%, respectively. Recoveries of 78.8 +/- 6.4% for B1-Lys and 85.4 +/- 12.4% for the internal standard were based on the full extraction and reconstitution processes. The method can be used to quantitate B1-Lys at the 0.5 pg/mg albumin level and is suitable for routine analysis. 相似文献