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131.
Engineering of efficient panchromatic sensitizers for nanocrystalline TiO(2)-based solar cells. 总被引:20,自引:0,他引:20
M K Nazeeruddin P Péchy T Renouard S M Zakeeruddin R Humphry-Baker P Comte P Liska L Cevey E Costa V Shklover L Spiccia G B Deacon C A Bignozzi M Gr?tzel 《Journal of the American Chemical Society》2001,123(8):1613-1624
A new series of panchromatic ruthenium(II) sensitizers derived from carboxylated terpyridyl complexes of tris-thiocyanato Ru(II) have been developed. Black dye containing different degrees of protonation [(C(2)H(5))(3)NH][Ru(H(3)tcterpy)(NCS)(3)] 1, [(C(4)H(9))(4)N](2)[Ru(H(2)tcterpy)(NCS)(3)] 2, [(C(4)H(9))(4)N](3)[Ru(Htcterpy)(NCS)(3)] 3, and [(C(4)H(9))(4)N](4)[Ru(tcterpy)(NCS)(3)] 4 (tcterpy = 4,4',4' '-tricarboxy-2,2':6',2' '-terpyridine) have been synthesized and fully characterized by UV-vis, emission, IR, Raman, NMR, cyclic voltammetry, and X-ray diffraction studies. The crystal structure of complex 2 confirms the presence of a Ru(II)N6 central core derived from the terpyridine ligand and three N-bonded thiocyanates. Intermolecular H-bonding between carboxylates on neighboring terpyridines gives rise to 2-D H-bonded arrays. The absorption and emission maxima of the black dye show a bathochromic shift with decreasing pH and exhibit pH-dependent excited-state lifetimes. The red-shift of the emission maxima is due to better pi-acceptor properties of the acid form that lowers the energy of the CT excited state. The low-energy metal-to-ligand charge-transfer absorption band showed marked solvatochromism due to the presence of thiocyanate ligands. The Ru(II)/(III) oxidation potential of the black dye and the ligand-based reduction potential shifted cathodically with decreasing number of protons and showed more reversible character. The adsorption of complex 3 from methoxyacetonitrile solution onto transparent TiO(2) films was interpreted by a Langmuir isotherm yielding an adsorption equilibrium constant, K(ads), of (1.0 +/- 0.3) x 10(5) M(-1). The amount of dye adsorbed at monolayer saturation was (n(alpha) = 6.9 +/- 0.3) x 10(-)(8) mol/mg of TiO(2), which is around 30% less than that of the cis-di(thiocyanato)bis(2,2'-bipyridyl-4,4'-dicarboxylate)ruthenium(II) complex. The black dye, when anchored to nanocrystalline TiO(2) films achieves very efficient sensitization over the whole visible range extending into the near-IR region up to 920 nm, yielding over 80% incident photon-to-current efficiencies (IPCE). Solar cells containing the black dye were subjected to analysis by a photovoltaic calibration laboratory (NREL, U.S.A.) to determine their solar-to-electric conversion efficiency under standard AM 1.5 sunlight. A short circuit photocurrent density obtained was 20.5 mA/cm(2), and the open circuit voltage was 0.72 V corresponding to an overall conversion efficiency of 10.4%. 相似文献
132.
Glen B. Deacon Penny R. Drago Dirk Gbbels Mathias S. Wickleder Gerd Meyer 《无机化学与普通化学杂志》2001,627(5):811-813
From the reaction of PtCl2(hex) (hex = hexa‐1,5‐diene) with LiC6F5 in diethyl ether, the complex [Pt{CH(CH2C6F5)CH2CH2CH=CH2}(C6F5)(OH2)] ( 1 ) was isolated. The crystal structure (monoclinic, C2/c (no. 15), Z = 8, a = 15.241(3), b = 16.579(2), c = 16.225(2) Å, β = 111.12(2)°) shows a complex with square planar coordination around platinum with a template formed 1‐pentafluorophenylhex‐5‐en‐2‐yl ligand, and C6F5 and aqua ligands trans to the double bond and alkyl carbon, respectively. 相似文献
133.
The X‐ray crystal structures of [PtCl2(dppm)], [Pt(C6F5)2L] (L = dppm (bis(diphenylphosphino)methane), dpam (bis(diphenylarsino)methane), dpae (bis(diphenylarsino)ethane)) and [PtCl(C6F5)(dpae)] show the complexes to be monomeric with chelating dipnictido ligands, and not alternatives with bridging ligands. In [Pt(C6F5)2(dpam)2], there are two unidentate diarsine ligands in a cis‐arrangement. 相似文献
134.
Zelakiewicz BS Lica GC Deacon ML Tong Y 《Journal of the American Chemical Society》2004,126(32):10053-10058
On 13C1-labeled octanethiol-protected 2.7 nm Pd nanoparticle surfaces, it has been observed that the 13C1 NMR of the alpha-carbon shows a peak centered around 38 ppm (with respect to tetramethylsilane (TMS)), which virtually coincides with that of the alpha-carbons in a dioctyl-disulfide molecule (39.3 ppm), and the corresponding 13C1 spin-spin relaxation becomes nonexponential. In addition, the infrared spectrum of the same sample shows that the ligands have a 100% gauche conformation, which is also consistent with a dioctyl-disulfide arrangement. By comparing with data obtained on 13C1-labeled octanethiol-protected 2.8 nm Au nanoparticles, we propose that a dioctyl-disulfide structure of the ligands is formed on the octanethiol-protected Pd nanoparticle surface, in contrast to the thiolate structure proposed on the Au nanoparticles. In addition, CO adsorption experiments show no sign of a PdS layer formed on the Pd nanoparticle surface. Furthermore, data taken over a period of more than 1 year show that the Pd nanoparticles are rather stable in organic solvents (for instance benzene), although slow degradation does happen and oxygen seems to play an important role in accelerating the degradation. 相似文献
135.
136.
137.
D. A. G. Deacon 《Applied Physics A: Materials Science & Processing》1979,19(1):97-104
A one-dimensional linearized analysis of a storage-ring laser is developed. The dynamic and equilibrium behavior of the energy
spread, bunch length, and correlation are derived analytically through a formalism generally applicable to linear difference
equations. The limits on the applicability of the linear approximation are discussed. 相似文献
138.
139.
K. E. Robinson D. A. G. Deacon J. M. J. Madey M. F. Velghe C. Bazin M. Bergher M. Billardon P. Elleaume J. M. Ortega Y. Petroff 《Applied physics. B, Lasers and optics》1985,36(1):41-52
This paper summarizes the basic low-current, laser-induced bunch-lengthening measurements that have been made on the ACO Storage-Ring Free-Electron Laser (SRFEL). The measurements provide verification of both the functional dependence and absolute magnitude of SRFEL theoretical models. The method of measurement, which is is explained, exploits frequency-domain techniques and is capable of accuracies comparable to those of a streak camara. The measurements are in good agreement with existing SRFEL theory and provide an important base for future work.Work supported in part by AFOSR under contract F49620-80-C-0068, the DGRST under contract 79-7-0163, and the DRET under contract 9-073 and 81-131 相似文献
140.
Only two preparations of pentafluorophenylorganometallics by sulphur dioxide elimination reactions have been reported. Thermal decomposition of the S-sulphinato complex C6F5SO2Fe(π-C5H5)(CO)2 gives C6F5Fe(π-C5H5)(CO)21, and a pentaflurophenyliridium compound has been prepared by the reaction2:IrCl(Ph3P)2N2 + C6F5SO2Cl→ C6F5IrCl2(Ph3P)2SO2 + N2 (1) 相似文献