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1.
A series of photoreactive complexes of the type Ru(terpy*)(N-N)(L)(2+), where terpy* is 4'-(3,5-ditertiobutylphenyl)-2,2':6',2' '-terpyridine, N-N is the bidentate chelate phen or dmp (phen = 1,10-phenanthroline, dmp = 2,9-dimethyl-1,10-phenanthroline), and L is the monodentate ligand dms, MeBN, or MeOBN (dms = dimethyl sulfide, MeBN = 2,6-dimethyl benzonitrile, MeOBN = 2,6-dimethoxybenzonitrile), has been synthesized and fully characterized by proton NMR spectroscopy, electrospray mass spectrometry, and UV-vis spectroscopy. The X-ray structures of four complexes were also obtained. In neat pyridine, the quantum yields for the photosubsitution of L by pyridine were measured and showed dramatic variations depending on the steric interactions between the spectator bidentate ligand and the leaving monodentate ligand L. The use of dmp instead of phen multiplied the photosubstitution efficiency by a factor of 20-50, depending on L. This effect could be qualitatively correlated to the distortions observed in the X-ray structures of the corresponding complexes. The highly distorted structure of Ru(terpy)(dmp)(dms)(PF(6))(2) showed a very high photosubsitution quantum yield phi = 0.36 in neat pyridine. The high photoreactivity of some of the compounds makes them particularly promising as components of future light-driven molecular machines. 相似文献
2.
The title sulfoxide 5 is worthy of interest because of its isoprenoid structure and its synthetic potentialities1 相似文献
3.
Our preceding studies have shown that lithio carbanions of protected cyanohydrins can undergo Michael additions to an isoprenic sulfoxide to yield lithio derivatives of allylic sulfoxides1. These results have led us to investigate the utilization of these lithio sulfoxides for new simple syntheses of aliphatic terpenes by head-to-tail linking of functionalized isoprenoid units. For this purpose, 1,2-epoxy-2-methyl-3-butene 2 was one especially appropriate electro-phile, but at the outset of our work, there had been very few investigations of the reactivity of lithio carbanions of allylic sulfoxides with epoxides2 相似文献
4.
Two-Photon-Induced CO-Releasing Molecules as Molecular Logic Systems in Solution,Polymers, and Cells
Dr. Vadde Ramu Dr. Gandra Upendar Reddy Dr. Jingjing Liu Patrick Hoffmann Dr. Rudrakant Sollapur Dr. Ralf Wyrwa Dr. Stephan Kupfer Prof. Dr. Christian Spielmann Dr. Sylvestre Bonnet Prof. Dr. Ute Neugebauer Dr. Alexander Schiller 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(36):8453-8458
Phototherapeutic applications of carbon monoxide (CO)-releasing molecules are limited because they require harmful UV and blue light for activation. We describe two-photon excitation with NIR light (800 nm)-induced CO-release from two MnI tricarbonyl complexes bearing 1,8-naphthalimide units ( 1 , 2 ). Complex 2 behaves as a logic OR gate in solution, nonwovens, and in HeLa cells. CO release, indicated by fluorescence enhancement, was detected in solution, nonwoven, and HeLa cells by single- (405 nm) and two-photon (800 nm) excitation. The photophysical properties of 1 and 2 have been measured and supported by DFT and TDDFT quantum chemical calculations. Both photoCORMs are stable in the dark in solution and noncytotoxic, leading to promising applications as phototherapeutics with NIR light. 相似文献
5.
We demonstrate efficient frequency conversion with large frequency shifts of an anti-Stokes signal into a parametrically seeded Stokes idler, which is generated by a highly mismatched three-wave mixing interaction and subsequent Raman amplification in a normally dispersive single-mode fiber. The use of non-phase-matched waves in Raman-assisted three-wave mixing interactions overcomes the strict spectral limitations imposed by phase-matching conditions in parametric frequency-conversion processes. 相似文献
6.
7.
Bonnet S Limburg B Meeldijk JD Gebbink RJ Killian JA 《Journal of the American Chemical Society》2011,133(2):252-261
Electrostatic forces play an important role in the interaction between large transition metal complexes and lipid bilayers. In this work, a thioether-cholestanol hybrid ligand (4) was synthesized, which coordinates to ruthenium(II) via its sulfur atom and intercalates into lipid bilayers via its apolar tail. By mixing its ruthenium complex [Ru(terpy)(bpy)(4)](2+) (terpy = 2,2';6',2'-terpyridine; bpy = 2,2'-bipyridine) with either the negatively charged lipid dimyristoylphosphatidylglycerol (DMPG) or with the zwitterionic lipid dimyristoylphosphatidylcholine (DMPC), large unilamellar vesicles decorated with ruthenium polypyridyl complexes are formed. Upon visible light irradiation the ruthenium-sulfur coordination bond is selectively broken, releasing the ruthenium fragment as the free aqua complex [Ru(terpy)(bpy)(OH(2))](2+). The photochemical quantum yield under blue light irradiation (452 nm) is 0.0074(8) for DMPG vesicles and 0.0073(8) for DMPC vesicles (at 25 °C), which is not significantly different from similar homogeneous systems. Dynamic light scattering and cryo-TEM pictures show that the size and shape of the vesicles are not perturbed by light irradiation. Depending on the charge of the lipids, the cationic aqua complex either strongly interacts with the membrane (DMPG) or diffuses away from it (DMPC). Back coordination of [Ru(terpy)(bpy)(OH(2))](2+) to the thioether-decorated vesicles takes place only at DMPG bilayers with high ligand concentrations (25 mol %) and elevated temperatures (70 °C). During this process, partial vesicle fusion was also observed. We discuss the potential of such ruthenium-decorated vesicles in the context of light-controlled molecular motion and light-triggered drug delivery. 相似文献
8.
Activation of a Photodissociative Ruthenium Complex by Triplet–Triplet Annihilation Upconversion in Liposomes 下载免费PDF全文
Sven H. C. Askes Azadeh Bahreman Dr. Sylvestre Bonnet 《Angewandte Chemie (International ed. in English)》2014,53(4):1029-1033
Liposomes capable of generating photons of blue light in situ by triplet–triplet annihilation upconversion of either green or red light, were prepared. The red‐to‐blue upconverting liposomes were capable of triggering the photodissociation of ruthenium polypyridyl complexes from PEGylated liposomes using a clinical grade photodynamic therapy laser source (630 nm). 相似文献
9.
It is shown that the title transformations occurred through basecatalyzed opening of the cyclopropane ring into the dienic nitrile which then reacted with the in situ formed formaldehyde to yield the bicyclic compound . 相似文献
10.
We numerically and experimentally report the observation of slow-light spatial solitons in a Kerr medium owing to light amplification by stimulated Raman scattering. This was achieved in a CS2 nonlinear planar waveguide that possesses both a strong self-focusing nonlinearity to generate the spatial Raman soliton and a Raman susceptibility sharp enough to induce the slow-light process simultaneously. We show that the Raman Stokes component is optically delayed by more than 120 ps for a 140 ps Raman pulse duration and only 3 cm of propagation length, while propagating as a spatial soliton beam. 相似文献