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21.
Maroto E Filippone S Martín-Domenech A Suárez M Martín N Martínez-Alvarez R 《Journal of mass spectrometry : JMS》2011,46(10):1016-1029
The mass spectra of new substituted pyrrolidino[60]- and [70]fullerenes have been obtained using electrospray ionization conditions in the positive and negative mode of detection with two different mass spectrometers, a quadrupole ion trap and a Fourier transform ion cyclotron resonance. Radical anions M(●-) and deprotonated molecules [M-H](-) are formed under negative electrospray ionization mass spectrometry conditions, and the collision-induced dissociations of both ionic species have been studied. Either negative odd-electron ions or negative even-electron ions undergo a retro-cycloaddition process forming the corresponding fullerene product ions C(60)(●-) and C(70)(●-). The generation of fullerene radical anions from deprotonated molecules is a new exception of the "even-electron rule." In contrast, the protonated molecules [M + H](+) obtained from the positive mode of detection do not undergo this cycloreversion reaction, and the MS(n) experiment reveals a variety of eliminations of neutral molecules involving different hydrogen shifts and multiple bond cleavages that lead eventually to substituted methanofullerene fragment ions. The observed fragmentations can be correlated with the electronic character of the substituents attached to the heterocyclic moiety. The results obtained from the thermal reactions of these compounds, carried out under different pH conditions, correlate well with those obtained in gas phase. The different behaviors between protonated and unprotonated molecules and ions can be explained assuming that the retro-cycloaddition reaction takes place only when the nitrogen atom of the pyrrolidine ring (the basic center of the molecule) is unprotonated both in gas and condensed phase. The protonation of the NH group inhibits the cycloreversion process, and therefore different fragmentations take place. The detailed mechanisms of the formation and evolution of the intermediate fragments are described. 相似文献
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B.D. Ganapol W.L. Filippone 《Journal of Quantitative Spectroscopy & Radiative Transfer》1982,27(1):15-21
The time-dependent emergent intensity for an arbitrarily anisotropically-scattering, semi-infinite medium is obtained in terms of the stationary collided intensities. A numerical example is presented for a Rayleigh scattering atmosphere. 相似文献
25.
Mattioli G Filippone F Giannozzi P Caminiti R Amore Bonapasta A 《Physical review letters》2008,101(12):126805
Metallo-organic molecules with highly conjugated pi-electrons, like phthalocyanines (Pc's), are widely investigated for usage in electronic and electro-optic devices. However, their weak coupling with semiconductors is an obstacle to technological applications. Here we report a first-principle theoretical study of some fundamental features of the Pc-semiconductor interaction. Our results shed light on the general problem of organic-inorganic coupling and show that an effective coupling can be achieved by a careful choice of the Pc-substrate system and the semiconductor doping. Our results also reveal a universal alignment of the Pc electronic levels to the semiconductor band gap and suggest a general procedure for designing efficiently coupled organic-inorganic systems. 相似文献
26.
Attanasi OA Favi G Filippone P Giorgi G Mantellini F Moscatelli G Spinelli D 《Organic letters》2008,10(10):1983-1986
The versatility of the Mukaiyama-Michael-type addition/heterocyclization of Danishefsky's diene with 1,2-diaza-1,3-butadienes was applied to the synthesis of both 4 H-1-aminopyrroles and 4,5 H-pyrazoles. Thus, the same reagents furnished different types of highly functionalized azaheterocycles essentially depending on their structure: as a matter of fact, R1 = COOR or CONR 2 differently affects the acidity of the proton at the adjacent carbon. An unexpected formation of 5 H-1-aminopyrroles from the reactions carried out in water was also observed. 相似文献
27.
Martín N Altable M Filippone S Martín-Domenech A Martínez-Alvarez R Suarez M Plonska-Brzezinska ME Lukoyanova O Echegoyen L 《The Journal of organic chemistry》2007,72(10):3840-3846
Isoxazolino[4,5:1,2][60]- and -[70]fullerenes undergo an efficient retro-cycloaddition reaction to pristine fullerene by thermal treatment in the presence of an excess of a dienophile and Cu(II) catalysis, which can be selectively used in the presence of malonate or pyrrolidine cycloadducts. Trapping experiments using N-phenylmaleimide as dipolarophile have shown that the reaction mechanism occurs by thermal removal of the nitrile oxide 1,3-dipole, in a process which is favored by the presence of Cu(II) as the catalyst. The ESI-MS study supports the observed retro-cycloaddition process for both C60 and C70 derivatives. In contrast to previous electrochemical retro-cycloaddition processes observed in fulleropyrrolidines, isoxazolinofullerenes were stable under oxidative conditions. 相似文献
28.
Orazio A. Attanasi Paolino Filippone Barbara Guidi Thomas Hippe Fabio Mantellini Lutz F. Tietze 《Tetrahedron letters》1999,40(52):827-9280
The first general protocol for the preparation of different polymer-bound 1,2-diaza-1,3-butadienes is reported. The utility of these supported reagents in the solid-phase synthesis of 4-triphenylphosphoranylidene-4,5-dihydropyrazol-5-ones by reaction with triphenylphosphine is presented. 相似文献
29.
Aparicio D Attanasi OA Filippone P Ignacio R Lillini S Mantellini F Palacios F de Los Santos JM 《The Journal of organic chemistry》2006,71(16):5897-5905
The preparation of tetrahydropyrazines, dihydropyrazines, pyrazines, piperazinones, and quinoxalines by 1,4-addition of 1,2-diamines to 1,2-diaza-1,3-butadienes bearing carboxylate, carboxamide, or phosphorylated groups at the terminal carbon and subsequent internal heterocyclization is described. The solvent-free reaction of carboxylated 1,2-diaza-1,3-butadienes with the same reagents affords piperazinones, while phosphorylated 1,2-diaza-1,3-butadienes yield phosphorylated pyrazines. The solid-phase reaction of polymer-bound 1,2-diaza-1,3-butadienes with 1,2-diamines produces pyrazines. 相似文献
30.
Fomin N Arrington J Asaturyan R Benmokhtar F Boeglin W Bosted P Bruell A Bukhari MH Christy ME Chudakov E Clasie B Connell SH Dalton MM Daniel A Day DB Dutta D Ent R El Fassi L Fenker H Filippone BW Garrow K Gaskell D Hill C Holt RJ Horn T Jones MK Jourdan J Kalantarians N Keppel CE Kiselev D Kotulla M Lindgren R Lung AF Malace S Markowitz P McKee P Meekins DG Mkrtchyan H Navasardyan T Niculescu G Opper AK Perdrisat C Potterveld DH Punjabi V Qian X Reimer PE Roche J Rodriguez VM Rondon O 《Physical review letters》2012,108(9):092502
We present new measurements of electron scattering from high-momentum nucleons in nuclei. These data allow an improved determination of the strength of two-nucleon correlations for several nuclei, including light nuclei where clustering effects can, for the first time, be examined. The data also include the kinematic region where three-nucleon correlations are expected to dominate. 相似文献