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101.
Since their introduction in image denoising, the family of non-local methods, whose Non-Local Means (NL-Means) is the most famous member, has proved its ability to challenge other powerful methods such as wavelet based approaches or variational techniques. Though simple to implement and efficient in practice, the classical NL-Means algorithm suffers from several limitations: noise artifacts are created around edges and regions with few repetitions in the image are not treated at all. In this paper, we present an easy to implement and time efficient modification of the NL-Means based on a better reprojection from the patches space to the original pixel space, specially designed to reduce the artifacts due to the rare patch effect. We compare the performance of several reprojection schemes on a toy example and on some classical natural images. 相似文献
102.
103.
Liu B Roisnel T Guégan JP Carpentier JF Sarazin Y 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(20):6289-6301
The factors governing the stability and the reactivity towards cyclic esters of heteroleptic complexes of the large alkaline earth metals (Ae) have been probed. The synthesis and stability of a family of heteroleptic silylamido and alkoxide complexes of calcium [{LO(i)}Ca-Nu(thf)(n)] supported by mono-anionic amino ether phenolate ligands (i = 1, {LO(1)}(-) = 4-(tert-butyl)-2,6-bis(morpholinomethyl)phenolate, Nu(-) = N(SiMe(2)H)(2)(-), n = 0, 4; i = 2, {LO(2)}(-) = 2,4-di-tert-butyl-6-{[2-(methoxymethyl)pyrrolidin-1-yl]methyl}phenolate, Nu(-) = N(SiMe(2)H)(2)(-), n = 0, 5; i = 4, {LO(4)}(-) = 2-{[bis(2-methoxyethyl)amino]methyl}-4,6-di-tert-butylphenolate, Nu(-) = N(SiMe(2)H)(2)(-), n = 1, 6; Nu(-) = HC≡CCH(2)O(-), n = 0, 7) and those of the related [{LO(3)}Ae-N(SiMe(2)H)(2)] ({LO(3)}(-) = 2-[(1,4,7,10-tetraoxa-13-azacyclopentadecan-13-yl)methyl]-4,6-di-tert-butylphenolate Ae = Ca, 1; Sr, 2; Ba, 3) have been investigated. The molecular structures of 1, 2, [(4)(2)], 6, and [(7)(2)] have been determined by X-ray diffraction. These highlight Ae???H-Si internal β-agostic interactions, which play a key role in the stabilization of [{LO(i)}Ae-N(SiMe(2)H)(2)] complexes against ligand redistribution reactions, in contrast to regular [{LO(i)}Ae-N(SiMe(3))(2)]. Pulse-gradient spin-echo (PGSE) NMR measurements showed that 1, 4, 6, and 7 are monomeric in solution. Complexes 1-7 mediate the ring-opening polymerization (ROP) of L-lactide highly efficiently, converting up to 5000?equivalents of monomer at 25?°C in a controlled fashion. In the immortal ROP performed with up to 100?equivalents of exogenous 9-anthracenylmethanol or benzyl or propargyl alcohols as a transfer agent, the activity of the catalyst increased with the size of the metal (1<2<3). For Ca-based complexes, the enhanced electron-donating ability of the ancillary ligand favored catalyst activity (1>6>4≈5). The nature of the alcohol had little effect over the activity of the binary catalyst system 1/ROH; in all cases, both the control and end-group fidelity were excellent. In the living ROP of L-LA, the HC≡CCH(2)O(-) initiating group (as in 7) proved superior to N(SiMe(2)H)(2)(-) or N(SiMe(3))(2)(-) (as in 6 or [{LO(4)}Ca-N(SiMe(3))(2)] (B), respectively). 相似文献
104.
105.
Gronnier C Kramer S Odabachian Y Gagosz F 《Journal of the American Chemical Society》2012,134(2):828-831
In the presence of a Cu(I) catalyst and a pyridine oxide, alkynyl oxiranes and oxetanes can be converted into functionalized five- or six-membered α,β-unsaturated lactones or dihydrofuranaldehydes. This new oxidative cyclization is proposed to proceed via an unusual allenyloxypyridinium intermediate. 相似文献
106.
Joosten A Trolez Y Collin JP Heitz V Sauvage JP 《Journal of the American Chemical Society》2012,134(3):1802-1809
A new copper-complexed [3]rotaxane consisting of two coordinating 30-membered rings threaded by a two-binding-site axis has been prepared in good yield from relatively simple organic fragments. The main specificity of the system originates from the stoppering reaction, based on "click" chemistry, and thus from the presence of two triazole groups at positions next to the bidentate chelates of the axis central part. The geometry of the coordinating atoms belonging to the axis is such that the triazole groups can either be part of the coordinating fragments when the metal center is 5-coordinate or be not at all involved in coordination to the metal when the latter is 4-coordinate. To be more specific, when the two complexed metal centers are monovalent copper(I) centers, the triazoles are not included in the metal coordination sphere, whereas when the metal centers are Cu(II) or Zn(2+), the triazole groups are bound to the metals. This is easily explained by the fact that Cu(I) is preferably 4-coordinate and Cu(II) and Zn(2+) are 5-coordinate. The interconversion between both situations (4- or 5-coordinate) can be quantitatively induced by metal exchange (Cu(I)/Zn(2+)) or by a redox process (Cu(II)/Cu(I)). It leads to important geometrical changes and in particular to a strong modification of the angle between the two rings. As a consequence, the two threaded rings undergo a motion which is reminiscent of a wing-flapping movement similar to that of birds. This flapping motion is fast and quantitative. It should lead to new functional molecular machines in the future. 相似文献
107.
Chavillon B Cario L Renaud A Tessier F Cheviré F Boujtita M Pellegrin Y Blart E Smeigh A Hammarström L Odobel F Jobic S 《Journal of the American Chemical Society》2012,134(1):464-470
Zinc oxide is considered as a very promising material for optoelectronics. However, to date, the difficulty in producing stable p-type ZnO is a bottleneck, which hinders the advent of ZnO-based devices. In that context, nitrogen-doped zinc oxide receives much attention. However, numerous reviews report the controversial character of p-type conductivity in N-doped ZnO, and recent theoretical contributions explain that N-doping alone cannot lead to p-typeness in Zn-rich ZnO. We report here that the ammonolysis at low temperature of ZnO(2) yields pure wurtzite-type N-doped ZnO nanoparticles with an extraordinarily large amount of Zn vacancies (up to 20%). Electrochemical and transient spectroscopy studies demonstrate that these Zn-poor nanoparticles exhibit a p-type conductivity that is stable over more than 2 years under ambient conditions. 相似文献
108.
FX Gallat AP Brogan Y Fichou N McGrath M Moulin M Härtlein J Combet J Wuttke S Mann G Zaccai CJ Jackson AW Perriman M Weik 《Journal of the American Chemical Society》2012,134(32):13168-13171
The observation of biological activity in solvent-free protein-polymer surfactant hybrids challenges the view of aqueous and nonaqueous solvents being unique promoters of protein dynamics linked to function. Here, we combine elastic incoherent neutron scattering and specific deuterium labeling to separately study protein and polymer motions in solvent-free hybrids. Myoglobin motions within the hybrid are found to closely resemble those of a hydrated protein, and motions of the polymer surfactant coating are similar to those of the hydration water, leading to the conclusion that the polymer surfactant coating plasticizes protein structures in a way similar to hydration water. 相似文献
109.
Dr. Bo Liu Dr. Thierry Roisnel Jean‐Paul Guégan Prof. Jean‐François Carpentier Dr. Yann Sarazin 《Chemistry (Weinheim an der Bergstrasse, Germany)》2012,18(20):6289-6301
The factors governing the stability and the reactivity towards cyclic esters of heteroleptic complexes of the large alkaline earth metals (Ae) have been probed. The synthesis and stability of a family of heteroleptic silylamido and alkoxide complexes of calcium [{LOi}Ca? Nu(thf)n] supported by mono‐anionic amino ether phenolate ligands (i=1, {LO1}?=4‐(tert‐butyl)‐2,6‐bis(morpholinomethyl)phenolate, Nu?=N(SiMe2H)2?, n=0, 4 ; i=2, {LO2}?=2,4‐di‐tert‐butyl‐6‐{[2‐(methoxymethyl)pyrrolidin‐1‐yl]methyl}phenolate, Nu?=N(SiMe2H)2?, n=0, 5 ; i=4, {LO4}?=2‐{[bis(2‐methoxyethyl)amino]methyl}‐4,6‐di‐tert‐butylphenolate, Nu?=N(SiMe2H)2?, n=1, 6 ; Nu?=HC?CCH2O?, n=0, 7 ) and those of the related [{LO3}Ae? N(SiMe2H)2] ({LO3}?=2‐[(1,4,7,10‐tetraoxa‐13‐azacyclopentadecan‐13‐yl)methyl]‐4,6‐di‐tert‐butylphenolate Ae=Ca, 1 ; Sr, 2 ; Ba, 3 ) have been investigated. The molecular structures of 1 , 2 , [( 4 )2], 6 , and [( 7 )2] have been determined by X‐ray diffraction. These highlight Ae???H? Si internal β‐agostic interactions, which play a key role in the stabilization of [{LOi}Ae? N(SiMe2H)2] complexes against ligand redistribution reactions, in contrast to regular [{LOi}Ae? N(SiMe3)2]. Pulse‐gradient spin‐echo (PGSE) NMR measurements showed that 1 , 4 , 6 , and 7 are monomeric in solution. Complexes 1 – 7 mediate the ring‐opening polymerization (ROP) of L ‐lactide highly efficiently, converting up to 5000 equivalents of monomer at 25 °C in a controlled fashion. In the immortal ROP performed with up to 100 equivalents of exogenous 9‐anthracenylmethanol or benzyl or propargyl alcohols as a transfer agent, the activity of the catalyst increased with the size of the metal ( 1 < 2 < 3 ). For Ca‐based complexes, the enhanced electron‐donating ability of the ancillary ligand favored catalyst activity ( 1 > 6 > 4 ≈ 5 ). The nature of the alcohol had little effect over the activity of the binary catalyst system 1 /ROH; in all cases, both the control and end‐group fidelity were excellent. In the living ROP of L ‐LA, the HC?CCH2O? initiating group (as in 7 ) proved superior to N(SiMe2H)2? or N(SiMe3)2? (as in 6 or [{LO4}Ca? N(SiMe3)2] ( B ), respectively). 相似文献
110.