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91.
A new analysis method for the short excited‐state lifetime measurement of photosensitive species in crystals is described. Based on photocrystallographic techniques, this method is an alternative to spectroscopic methods and is also valid for non‐luminescent excited species. Two different approaches are described depending on the magnitude of the lifetime τ. For very short lifetimes below the width of the synchrotron pulse, an estimated τ can be obtained from the occurrence of the maximal system response as a function of the pump–probe delay time Δt. More precise estimates for both short and longer lifetimes can be achieved by a refinement of a model of the response as a function of the pump–probe delay time. The method also offers the possibility of the structure determination of excited species with lifetimes in the 40–100 ps range. 相似文献
92.
93.
O. Saengsawang A. Schüring T. Remsungnen S. Hannongbua D.A. Newsome A.J. Dammers M.O. Coppens S. Fritzsche 《Chemical physics》2010
The extremely slow diffusion of the molecule n-pentane caused by the hopping from cage-to-cage in zeolite ZK5 has been investigated by transition state theory (TST). Such slow diffusion cannot be accessed by usual molecular dynamics simulation techniques. The calculation of the partition function ratio needed for TST was enabled by a recently developed method, the so-called high-temperature configuration-space exploration (HTCE). Dynamical corrections for recrossing events have also been taken into account. The obtained intra-zeolite self-diffusion constant between 247 and 317 K of 10−16–10−15 m2 s−1 falls in the range of 10−18–10−15 m2 s−1 observed experimentally. The calculated energetic barrier between two neighboring cages of 29 kJ mol−1 is in good agreement with that of 28 ± 5 kJ mol−1 obtained from NMR measurement. 相似文献
94.
Jarosław A. Kalinowski Bertrand Fournier Anna Makal Philip Coppens 《Journal of synchrotron radiation》2012,19(4):637-646
A spot‐integration method is described which does not require prior indexing of the reflections. It is based on statistical analysis of the values from each of the pixels on successive frames, followed for each frame by morphological analysis to identify clusters of high value pixels which form an appropriate mask corresponding to a reflection peak. The method does not require prior assumptions such as fitting of a profile or definition of an integration box. The results are compared with those of the seed‐skewness method which is based on minimizing the skewness of the intensity distribution within a peak's integration box. Applications in Laue photocrystallography are presented. 相似文献
95.
A new cyclic gold(I) triazolate trimer, [Au(3,5-i-Pr2Tz)]3 (1), exhibits fully overlapping aurophilically bonded dimer-of-trimer units that lead to multiple phosphorescence bands in both the solid state and solution. The conformation of the hexanuclear unit exhibits reversible interconversion between C2 and D3 effective symmetries, depending on the crystal temperature or solution concentration, the variation of which leads to isoemissive and isosbestic points. Solutions of 1 exhibit remarkable quenching properties that demonstrate molecular recognition with high selectivity and hypersensitivity for some reagents, as influenced by protonation via Br?nsted acids, pi intercalation, and/or energy transfer. The quenched phosphorescence of 1 by acetic acids can be regenerated by NEt3. 相似文献
96.
97.
David Newsome Sofranita Gunawan Gino Baron Joeri Denayer Marc-Olivier Coppens 《Adsorption》2014,20(1):157-171
Zeolite crystals with cations present, such as ZSM-5, are widely used for gas sequestration, separations, and catalysis. One possible application is as an adsorbent to separate CO2 from N2 in flue gas mixtures. Typically, the zeolite framework is of a SiO2 composition, but tetravalent Si atoms can be replaced with trivalent Al atoms. This change in valence creates a charge deficit, requiring cations to maintain the charge balance. Experimental studies have demonstrated that cations enhance adsorption of polar molecules due to strong electrostatic interactions. While numerous adsorption studies have been performed for silicalite-1, the all-silica form of ZSM-5, fewer studies on ZSM-5 have been performed. Grand Canonical Monte Carlo simulations were used to study adsorption of CO2 and N2 in Na–ZSM-5 at T = 308 K, which is ZSM-5 with Na+ counter-ions present. The simulations suggest that a lower Si/Al ratio (or higher Na+ and Al content) substantially increases adsorption at low pressures. At high pressures, however, the effect of the Al substitutions is minor, because the Al?/Na+ sites are saturated with guest molecules. Similarly, a lower Si/Al ratio also increases the isosteric heat of adsorption at low loading, but the isosteric heats approach the silicalite-1 reference values at higher loadings. Comparison of simulations and experimental measurements of the adsorption isotherms and isosteric heats points to the importance of carefully considering the role of charge on the Na+ cations, and suggest that the balancing cations in ZSM-5, here Na+, only have partial charges. 相似文献
98.
There is a natural restriction on special divisors of a smooth projective curve C the Clifford index of C. In this paper we look for curves of Clifford index c on which all special divisors exist which are not prevented by c, and we construct two non-trivial examples for c = 4 and c = 5, respectively.
Received: 2 May 2005 相似文献
99.
100.
We present the three-loop calculation of the effective potential forλφ 4 in 3+1 dimensions, based on a new variational approach to quantum field theory. This formulation is based on a 2PPI loop expansion of an effective action for local composite operators and yields non-perturbative results. Renormalisation is carried out for both the trivial and the precarious phase using dimensional regularisation. The three-loop result is seen to be similar to the one-loop result (which coincides with the G.E.P.) and only one numerical constant in the effective potential has to be changed. 相似文献