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101.
G.?GusmanoEmail author R.?Montanari S.?Kaciulis G.?Montesperelli R.?Denk 《Applied Physics A: Materials Science & Processing》2004,78(2):205-211
Femtosecond laser induced adsorption site changes of CO at nanoparticulate palladium aggregates have been investigated using laser light at =400 nm and pulse lengths of 70 fs. The average sizes of the aggregates grown by evaporating palladium atoms onto an epitaxial Al2O3 film on NiAl(110) were varied between 100 and 6000 atoms per island. Amorphous aggregates grown at 120 K and crystalline aggregates grown at 300 K have been investigated. Beyond laser-induced migration of CO already reported for nanosecond experiments, adsorbate-induced surface roughening is apparent from Fourier-transform infrared reflection absorption spectroscopy. The laser-induced processes are correlated to the presence of higher local adsorbate densities and a substantial population of edge sites. A model is suggested attributing surface roughening to the formation of local hot spots after coherent electronic excitation via heating through highly vibrationally excited adsorbate states and energetic channelling along chains of elevated local adsorbate densities. The processes are most efficient for intermediate aggregate sizes. In contrast to nanosecond experiments, a few percent of CO molecules are desorbed during the femtosecond experiments from smaller aggregates. PACS 82.53.St 相似文献
102.
We develop an analytic approach for the study of lattice heteropolymers and apply it to copolymers with correlated Markovian sequences. According to our analysis, heteropolymers present three different dense phases depending upon the temperature, the nature of the monomer interactions, and the sequence correlations: (i) a liquid phase, (ii) a "soft glass" phase, and (iii) a "frozen glass" phase. The presence of the intermediate "soft glass" phase is predicted, for instance, in the case of polyampholytes with sequences that favor the alternation of monomers. Our approach is based on the cavity method, a refined Bethe-Peierls approximation adapted to frustrated systems. It amounts to a mean-field treatment in which the nearest-neighbor correlations, which are crucial in the dense phases of heteropolymers, are handled exactly. This approach is powerful and versatile; it can be improved systematically and generalized to other polymeric systems. 相似文献
103.
Salla I Montanari T Salagre P Cesteros Y Busca G 《The journal of physical chemistry. B》2005,109(2):915-922
The low temperature adsorption of CO and the room temperature adsorption of acetonitrile, propionitrile, isobutyronitrile, pivalonitrile, benzonitrile, and o-toluonitrile on Na-mordenite (NaMOR) have been investigated by Fourier transform infrared (FT-IR) spectroscopy. The results have been compared with analogous experiments performed on H-mordenite, Na-X zeolite, and Na-silica-alumina. The Na distribution in NaMOR has also been investigated by X-ray diffraction and far-IR spectroscopy. The conclusions are that Na+ ion distribution is essentially random and that, together with the well-known interaction of the probes with Na+ ions in the side pockets and the main channels, a stronger additional interaction occurs in all cases. This new interaction is likely multiple, involving either more Na+ ions or Na and oxygen species. This interaction is more pronounced with the hindered nitriles, whose access at the main channels is likely forbidden. This suggests that this interaction, which is also observed on Na-X zeolites but not with Na-silica-alumina, occurs at the external mouths of the mordenite channels. 相似文献
104.
Montanari T Herrera Delgado MC Bevilacqua M Busca G Larrubia Vargas MA Alemany LJ 《The journal of physical chemistry. B》2005,109(2):879-883
The interaction of triethoxysilane (TES) with H-ferrierite (H-FER) and its effects on acidity have been investigated by infrared spectroscopy. TES adsorbs only on the external surface of H-FER and allows the almost complete disappearance of the external silanol groups. New SiH groups are formed which appear to be inactive in acid-base interactions. The adsorption of propionitrile, which diffuses into the zeolitic channels, provides evidence for the lack of substantial perturbation of the strongly acidic internal bridging OH groups. On the contrary, the adsorption of the hindered basic probe molecule o-toluonitrile, which cannot penetrate the FER channels, shows that not only terminal silanols but also Al3+ Lewis acid sites present on the external surface of H-FER almost totally disappear after TES treatment. Treatment with TES seems to allow virtually the total deactivation of the H-FER external surface. 相似文献
105.
Randomized search algorithms for hard combinatorial problems exhibit a large variability of performances. We study the different types of rare events which occur in such out-of-equilibrium stochastic processes and we show how they cooperate in determining the final distribution of running times. As a by-product of our analysis we show how search algorithms are optimized by random restarts. 相似文献
106.
We consider the dynamics of a diluted mean-field spin glass model in the aging regime. The model presents a particularly rich heterogeneous behavior. In order to catch this behavior, we perform a spin-by-spin analysis for a given disorder realization. We confirm the connection between statics and dynamics at the level of single degrees of freedom. Moreover, working with single-site quantities, we can introduce a new response-vs-correlation plot, which clearly shows how heterogeneous degrees of freedom undergo coherent structural rearrangements. We discuss the general scenario which emerges from our work and (possibly) applies to more realistic glassy models. Interestingly enough, some features of this scenario can be understood recurring to thermometric considerations. 相似文献
107.
Marco Berettoni Rinaldo Marini Bettolo Vittorio Montanari Teresa Prencipe Sergio Romeo 《Helvetica chimica acta》1991,74(8):1671-1678
Methods for a stereoselective preparation of compounds of type 2b , a key intermediate of a previous synthesis of the tetracyclic diterpene stemarin ( la ), have been tested on model compounds 5a, 5c , and 8a . Thus, (±)-(1RS,6SR,8SR,11SR)-hydroxytricyclo[6.2.2.0l,6]dodecan-9-one ( 5a ) was transformed by the Mitsunobu reaction into (±)-(1RS,6SR,8SR,11RS)-11-(benzoyloxy)tricyclot[6.2.2.01,6]dodecan-9-one ( 6b ; Scheme 2). The latter was also obtained from (±)-(1RS,6SR,8SR,11RS)-11-[(4)-toluenesulfonyloxy]tricyclo[6.2.2.01,6]dodecan-9-one ( 5c ) by the action of Et4N (PhCOO) in acetone. Compound 6b was then converted into (±)-(1RS,6RS,8RS,9RS)-tricyclo[6.2.2.01,6]dodecan-9-ol ( 8b ), a model for 2b . Compound 8b was also prepared from its epimer 8a by the Mitsunobu reaction via ester 7b . The inversion of configuration of bicyclo[2.2.2]octan-2-ols or derivates was not previously described. The model studies paved the way to the diastereoselective synthesis of (+)-18-deoxystemarin ( 1b ) via 12β-hydroxy-13-methyl-9β,13β-ethano-9β-podocarpan-15-one ( 10a ) and 13-methyl-9β,13β-ethano-9β-podpcarpan-12α-ol ( 11b ). 相似文献
108.
Bianca Montanari Sidney J.L. Ribeiro Gaël Poirier Máximo S. Li 《Applied Surface Science》2008,254(17):5552-5556
Thin films were prepared using glass precursors obtained in the ternary system NaPO3BaF2WO3 and the binary system NaPO3WO3 with high concentrations of WO3 (above 40% molar). Vitreous samples have been used as a target to prepare thin films. Such films were deposited using the electron beam evaporation method onto soda-lime glass substrates. Several structural characterizations were performed by Raman spectroscopy and X-ray Absorption Near Edge Spectroscopy (XANES) at the tungsten LI and LIII absorption edges. XANES investigations showed that tungsten atoms are only sixfold coordinated (octahedral WO6) and that these films are free of tungstate tetrahedral units (WO4). In addition, Raman spectroscopy allowed identifying a break in the linear phosphate chains as the amount of WO3 increases and the formation of POW bonds in the films network indicating the intermediary behavior of WO6 octahedra in the film network. Based on XANES data, we suggested a new attribution of several Raman absorption bands which allowed identifying the presence of WO− and WO terminal bonds and a progressive apparition of WOW bridging bonds for the most WO3 concentrated samples (above 40% molar) attributed to the formation of WO6 clusters. 相似文献
109.
Maria Luiza C. Montanari Adriano D. Andricopulo Carlos A. Montanari 《Analytica chimica acta》2005,545(1):33-45
Chiral sulfoxide drugs such as omeprazole, lansoprazole and pantoprazole were chromatographed on three chiral stationary phases (CSP), using amylose tris-(phenylcarbamate) derivatives in the reversed-phase mode. The retention factors (k) and chromatographic partition coefficients (kw), obtained by extrapolation of the first according to the linear Snyder equation, were analyzed employing molecular interaction fields (MIF) of eluted analytes. Based on the generated MIF, chiral selectors could be identified for improving enantiomeric separation performance of the respective sulfoxides. The method is useful for predicting the complementarities between CSP and analytes, and thus to help the selection of appropriate stationary phases prior to their preparation. 相似文献
110.
Guido RV Oliva G Montanari CA Andricopulo AD 《Journal of chemical information and modeling》2008,48(4):918-929
The glycolytic enzyme glyceraldehyde-3-phosphate dehydrogenase (GAPDH) is as an attractive target for the development of novel antitrypanosomatid agents. In the present work, comparative molecular field analysis and comparative molecular similarity index analysis were conducted on a large series of selective inhibitors of trypanosomatid GAPDH. Four statistically significant models were obtained ( r2 > 0.90 and q2 > 0.70), indicating their predictive ability for untested compounds. The models were then used to predict the potency of an external test set, and the predicted values were in good agreement with the experimental results. Molecular modeling studies provided further insight into the structural basis for selective inhibition of trypanosomatid GAPDH. 相似文献