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31.
Coverage‐ and Temperature‐Dependent Metalation and Dehydrogenation of Tetraphenylporphyrin on Cu(111)
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Michael Röckert Matthias Franke Quratulain Tariq Stefanie Ditze Michael Stark Patrick Uffinger Daniel Wechsler Upendra Singh Dr. Jie Xiao Dr. Hubertus Marbach Prof. Dr. Hans‐Peter Steinrück Dr. Ole Lytken 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(29):8948-8953
Using temperature‐programmed desorption, supported by X‐ray photoelectron spectroscopy and scanning tunneling microscopy, a comprehensive overview of the main reactions of 5,10,15,20‐tetraphenyl‐21H,23H‐porphyrin (2HTPP) on Cu(111) as a function of coverage and temperature is obtained. Three reactions were identified: metalation with Cu substrate atoms, stepwise partial dehydrogenation, and finally complete dehydrogenation. At low coverage the reactions are independent of coverage, but at higher coverage metalation becomes faster and partial dehydrogenation slower. This behavior is explained by a weaker interaction between the iminic nitrogen atoms and the Cu(111) surface in the high‐coverage checkerboard structure, leading to faster metalation, and the stabilizing effect of T‐type interactions in the CuTPP islands formed at high coverage after metalation, leading to slower dehydrogenation. Based on the amount of hydrogen released and the appearance in STM, a structure of the partially dehydrogenated molecule is suggested. 相似文献
32.
Ralph Weissleder David D. Stark Guillermo Elizondo Peter F. Hahn Carolyn Compton Sanjay Saini Jack Wittenberg Joseph T. Ferrucci 《Magnetic resonance imaging》1988,6(6):675-681
Thirteen patients with biopsy proven hepatic lymphoma (2 Hodgkin, 11 Non-Hodgkin) and a control group of 15 patients with hepatic metastases were analyzed quantitatively and qualitatively by MRI. Focal hepatic lymphoma was most reliably detected (eight of eight patients) and appeared hypointense relative to liver on T1 weighted (CNR − 7.4 ± 2.3) and hyperintense on T2 weighted (CNR + 8.4 ± 2.9) images. The mean T1 and T2 relaxation times of focal hepatic lymphoma (T1 = 832 ± 234 msec, T2 = 84 ± 16 ms) differed significantly from adjacent non-tumorous liver (T1 = 420 ± 121 ms, T2 = 51 ± 9 ms; p < 0.05), however CNR values and relaxation times were similar to those of hepatic metastases. Diffuse hepatic lymphoma (microscopic periportal infiltration) was undetectable by MRI in three patients by either morphologic features or quantitative criteria. A mixed pattern of hepatic lymphoma (focal lesions and diffuse infiltration) showed focal areas of slightly decreased signal intensity on T1 weighted images (CNR = −1.7 ± 0.4) while T2 weighted images revealed multiple regions of focal hyperintensity (CNR = +13.3 ± 8.4) superimposed on a diffusely hyperintense liver. Our experience demonstrates that either T1 or T2 weighted techniques are useful in detecting focal and that T2 weighted techniques are useful in detecting mixed hepatic lymphoma. Conventional image derived relaxation time measurements and quantitative parameters were of no additional diagnostic value. 相似文献
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34.
The fractionation technique described in this paper was used to characterize the melting-point, monomer, and blocking distributions for polymers and copolymers. It is different from the molecular-weight fractionation technique in that the fractions are obtained by using a single solvent to extract the solid polymer below its melting point at stepwise-increasing temperatures. The reproducibility of this technique is excellent, and the technique is sufficient to distinguish pellet-to-pellet variation in a commercially available polypropylene. It was used to show the influence of preparation variables on the melting-point distributions of polyethylene and polypropylene and on the monomer and blocking distribution of copolymers, and to distinguish copolymers from blends. 相似文献
35.
36.
Carretero-Gonzalez R Orstavik S Huke J Broomhead DS Stark J 《Chaos (Woodbury, N.Y.)》1999,9(2):466-482
The computation of the entire Lyapunov spectrum for extended dynamical systems is a very time consuming task. If the system is in a chaotic spatio-temporal regime it is possible to approximately reconstruct the Lyapunov spectrum from the spectrum of a subsystem by a suitable rescaling in a very cost effective way. We compute the Lyapunov spectrum for the subsystem by truncating the original Jacobian without modifying the original dynamics and thus taking into account only a portion of the information of the entire system. In doing so we notice that the Lyapunov spectra for consecutive subsystem sizes are interleaved and we discuss the possible ways in which this may arise. We also present a new rescaling method, which gives a significantly better fit to the original Lyapunov spectrum. We evaluate the performance of our rescaling method by comparing it to the conventional rescaling (dividing by the relative subsystem volume) for one- and two-dimensional lattices in spatio-temporal chaotic regimes. Finally, we use the new rescaling to approximate quantities derived from the Lyapunov spectrum (largest Lyapunov exponent, Lyapunov dimension, and Kolmogorov-Sinai entropy), finding better convergence as the subsystem size is increased than with conventional rescaling. (c) 1999 American Institute of Physics. 相似文献
37.
A simple synthesis of 28 new 6-alkyl- and 5,6-cycloalkeno-5-deazapteridines, also referred to as pyrido[2′,3′-d]pyrimidines, is described. 4-Aminouracils with various substituents at position 2 and N,N-unsubstituted β-enaminocarbonyl compounds such as 3-aminoacroleins and 2-aminomethylenecycloalkanones are the starting materials. The method is also applied to the preparation of terpenoid 5-deazapteridines from 2-aminomethylene terpene ketones. The fragmentation pattern of these heterocycles in the mass spectra is outlined, and the proton and carbon-13 NMR spectra are discussed. 相似文献
38.
Experiments by Gittings, Bandyopadhyay and Durian (Europhys. Lett. 65, 414 (2004)) demonstrate that light possesses a higher probability to propagate in the liquid phase of a foam due to total
reflection. The authors term this observation photon channelling which we investigate in this article theoretically. We first
derive a central relation in the work of Gitting et al. without any free parameters. It links the photon's path-length fraction f in the liquid phase to the liquid fraction ɛ. We then construct two-dimensional Voronoi foams, replace the cell edges by
channels to represent the liquid films and simulate photon paths according to the laws of ray optics using transmission and
reflection coefficients from Fresnel's formulas. In an exact honeycomb foam, the photons show superdiffusive behavior. It
becomes diffusive as soon as disorder is introduced into the foams. The dependence of the diffusion constant on channel width
and refractive index is explained by a one-dimensional random-walk model. It contains a photon channelling state that is crucial
for the understanding of the numerical results. At the end, we shortly comment on the observation that photon channelling
only occurs in a finite range of ɛ. 相似文献
39.
Observations in space and laboratory plasmas suggest magnetic reconnection as a mechanism for ion heating and formation of non-Maxwellian ion velocity distribution functions (IVDF). Laser-induced fluorescence measurements of the IVDF parallel to the X line of a periodically driven reconnection experiment are presented. A time-resolved analysis yields the evolution of the IVDF within a reconnection cycle. It is shown that reconnection causes a strong increase of the ion temperature, where the strongest increase is found at the maximum reconnection rate. Monte Carlo simulations demonstrate that ion heating is a consequence of the in-plane electric field that forms around the X line in response to reconnection. 相似文献
40.