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31.
H. Kurreck S. Aguirre H. Dieks J. Gtschmann J. v. Gersdorff H. Newman H. Schubert M. Speck T. Stabingis J. Sobek P. Tian A. Wiehe 《Radiation Physics and Chemistry》1995,45(6):853-865
Porphyrin quinones (P-Qs), covalently linked via different aliphatic bridges, have been synthesized and studies in their (porphyrin) cationic and (semiquinone) anionic radical states by EPR, ENDOR and TRIPLE resonance techniques. Electron transfer (ET) from the porphyrin donor to the quinone acceptor could be observed by time-resolved picosecond fluorescence spectroscopy (singlet ET) and by time-resolved EPR spectroscopy (triplet ET) in isotropic fluid solution and in anisotropic media (liquid crystals and reversed micelles). Steady-state in situ photoexcitation of P-Qs in CTAB cationic reversed micelles yielded the corresponding semiquinone radical anions. In TRITON X-100 reversed micelles both the radical cation of the porphyrin and the radical anion of the semiquinone could be detected, which occured in complete emission. In covalently linked porphyrin flavins ET from the photoexcited porphyrin fragment to the flavin and, in addition, energy transfer from the photoexcited flavin to the porphyrin could be observed. 相似文献
32.
G. Goll H. v. Löhneysen U. Kreibig G. Schmid 《Zeitschrift für Physik D Atoms, Molecules and Clusters》1991,20(1):329-331
Specific-heat measurements on the cluster compound Au55(P(C6H5)3)12Cl6 at temperatures 0.06 K ≤T≤3 K and in magnetic fields 0≤B≤6 T are reported. While above 0.6 K the specific heatC is dominated by the inter-cluster vibrational contribution observed previously, an anomalous increase ofC towards lowT is observed below 0.3 K, withC ~T ?2. This contribution develops into a Schottky-like anomaly forB≥0.4 T, indicating that it might be attributed to local moments which are also observed in ESR measurements. From the height of the anomaly one can infer that approximately one tenth of the Au55 clusters carry a magnetic moment. For 0.6 K≤T≤1 K andB=0 our data indicate the absence of a linear electronic specific-heat contribution expected for bulk Au. This possibly constitutes the first direct observation of the quantum-size effect on electronic energy levels in the specific heat. 相似文献
33.
Résumé Une étude théorique ab initio SCF-LCAO-MO de la méthylène imine et de l'anion vinyle a été effectuée. Les barrières d'énergie calculées pour l'inversion de l'azote et pour la rotation autour de la liaison C=N sont respectivement de 26–28 kcal/mole et de 57 kcal/mole.La barrière d'inversion du carbanion calculée pour l'anion vinyle est de 39 kcal/mole et l'isomérisation des imines se fait donc par inversion de l'azote. Les anions vinyliques ont une configuration stable.L'origine physique de ces barrières d'inversion est étudiée et caractérisée par les variations des termes énergétiques, de la composition de l'OM du doublet libre et des populations électroniques.La comparaison des processus d'inversion du carbanion, de l'azote et de l'oxonium dans la série CH2=CH, CH2=NH et CH2=OH a permis de mettre en évidence l'évolution des termes énergétiques, de la hauteur de la barrière et des transferts de population.
Précédent article de cette série: cf. Réf. [1].
Laboratoire associé au C.N.R.S. 相似文献
Theoretical conformational analysisIV. An ab initio SCF-LCAO-MO study of methylenimine and of vinyl anion
An ab initio SCF-LCAO-MO study of methylenimine and vinyl anion has been performed. The calculated barriers to nitrogen inversion and to rotation about the C=N bond are equal to 26–28 kcal/mole and 57 kcal/mole respectively.The calculated barrier to carbanion inversion in the vinyl anion amounts to 39 kcal/mole. Thus isomerization of imines occurs by a nitrogen inversion process and vinyl anions are configurationally stable.The physical origin of these inversion barriers is studied and characterized by the changes in the energy terms, in lone pair MO composition, and in electron populations.Comparison of the carbanion, nitrogen and oxonium inversion processes in the isoelectronic series CH2=CH, CH2=NH and CH2=OH permits to delineate general trends in the energy terms, barrier height and population transfers.
Zusammenfassung Für Methylenimin und das Vinylanion wird eine ab initio SCF-LCAO-MO-Studie durchgeführt. Die berechneten Barrieren für die Stíckstoffinversion und die Rotation um die C=N-Bindung betragen 26–28 kcal/Mol bzw. 57 kcal/Mol.Die berechnete Barriere für die Inversion des Carbanions im Vinylanion beträgt 39 kcal/Mol. Daher wird die Isomerisation von Iminen durch einen Stickstoffinversionsprozeß hervorgerufen, und die Konfigurationen von Vinyl-Anionen sind stabil.Der physikalische Ursprung dieser Inversionsbarrieren wird studiert und durch Änderungen in den Energietermen, in der Zusammensetzung von Ione pair-MO's und in den Besetzungszahlen der Elektronen charakterisiert.Ein Vergleich der Inversionsprozesse des Carbanions, des Stickstoffs und des Oxonium-Ions in der isoelektronischen Reihe CH2=CH–, CH2=NH and CH2=OH+ ermöglicht es, allgemeine Züge in den Energietermen, in den Höhen der Barrieren und den Besetzungsübergängen abzuleiten.
Précédent article de cette série: cf. Réf. [1].
Laboratoire associé au C.N.R.S. 相似文献
34.
The condensation of 1,5-diaminoimidazoles with ethyl aceto-acetate gives two types of compounds: imidazo[1,5-b]-1,2,4-triazepinones and imidazo[4,5-b]pyridinones. The structure of these compounds is demonstrated by rmn and mass spectroscopy. The formation of imidazo[4,5-b]pyridinones from imidazo[1,5-b]-triazepinones through a new transposition is also shown. 相似文献
35.
K. Freyer H. C. Treutler G. Just H. v. Philipsborn 《Journal of Radioanalytical and Nuclear Chemistry》2003,257(1):129-132
The online measurements of radon in flowing water with high temporal resolution and a lower limit of detection of some Bq/l is of growing interest in environmental research and earth sciences. Promising new fields of application in hydrogeology are the study of exchange and mixing processes and the monitoring of pumping procedures before and during groundwater sampling. A suitable, simple method has been proposed by Surbeck based on the separation of air and water by a diffusion membrane. Process parameters influencing the temporal resolution as well as the radon detection efficiency have been studied. Considering these results a new instrument has been developed enabling online radon-in-water measurement with time resolution of about one minute. 相似文献
36.
A. S. Aynacioglu A. -H. Meißner F. Walachowicz G. v. Oppen 《Zeitschrift für Physik D Atoms, Molecules and Clusters》1991,18(1):85-91
The magnetic depolarization of the impact radiation at λ(41 D?21 P)=492 nm and λ(31 D?21 P) = 668 nm as well as the splitting of the magnetic depolarisation signals in electric fields were investigated for 10–25 keV H 2 + (D 2 + )-He collisions (only 492 nm line) and for 5-22.5 keV He-He collisions (both lines). The results are compared with analogous measurements for He+- He and Ne+ - He collisions and the dynamics of the excitation process are qualitatively discussed. In particular, we emphasize the importance of inertia for the evolution of the electron cloud during the final phase of the collision process. 相似文献
37.
38.
The microstructures of four commercial linear low density polyethylenes (LLDPE) were evaluated and correlated with their sealing properties. Atomic Force Microscopy (AFM), Temperature Rising Elution Fractionation (TREF), Differential Scanning Calorimetry (DSC) and Crystallization Analysis Fractionation (CRYSTAF) experiments revealed that the comonomer distribution is one of the main factors that influence the sealing properties. The superior sealing performance showed by metallocene LLDPE samples in comparison to Ziegler-Natta LLDPE samples can be attributed to their well balanced chemical composition distribution. 相似文献
39.
We use a mathematical isomorphism between the one-dimensional exclusion process and the two-dimensional stochastic Ising model in the low-temperature limit to describe the typical instantaneous shape of a supercritical droplet. We derive, specifically, the exact asymptotic distribution of the boundaries of a (+1) spin region, confined to Z
+
2
and subjected to a positive magnetic field. In an appropriate scaling, the boundary distribution converges to a deterministic continuum limit.On leave at the EPFL, CH-1015 Lausanne, Switzerland. 相似文献
40.
K. Schiffer A. Dewald A. Gelberg R. Reinhardt K. O. Zell Sun Xianfu P. v. Brentano 《Zeitschrift für Physik A Hadrons and Nuclei》1986,325(4):487-488
The K=3/2 1 T rotational band has been identified in99Y with a band-head energy of 536 keV. This result is in contradiction with previously reported data, but is in agreement with predictions of the IBFM/PTQM model. 相似文献