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81.
We derive structure-property relationships for methine ("Brooker") dyes relating the color of the dye and its symmetric parents to its bond alternation in the ground state and also to the dipole properties associated with its low-lying charge-resonance (or charge-transfer) transition. We calibrate and test these relationships on an array of different protonation states of the green fluorescent protein chromophore motif (an asymmetric halochromic methine dye) and its symmetric parent dyes. The relationships rely on the assumption that the diabatic states that define the Platt model for methine dye color [J. R. Platt, J. Chem. Phys. 25, 80 (1956)] can also be distinguished by their single-double bond alternation and by their charge localization character. These assumptions are independent of the primary constraint that defines the diabatic states in the Platt model--specifically, the Brooker deviation rule for methine dyes [L. G. S. Brooker, Rev. Mod. Phys. 14, 275 (1942)]. Taking these assumptions, we show that the Platt model offers an alternate route to known structure-property relationships between the bond length alternation and the quadratic nonlinear polarizability β. We show also that the Platt model can be parameterized without the need for synthesis of the symmetric parents of a given dye, using the dipole data obtained through spectroscopic measurements. This suggests that the Platt model parameters may be used as independent variables in free-energy relationships for chromophores whose symmetric parents cannot be synthesized or chromophores strongly bound to biomolecular environments. The latter category includes several recently characterized biomolecular probe constructs. We illustrate these concepts by an analysis of previously reported electroabsorption and second-harmonic generation experiments on green fluorescent proteins. 相似文献
82.
83.
Churchard AJ Banach E Borgschulte A Caputo R Chen JC Clary D Fijalkowski KJ Geerlings H Genova RV Grochala W Jaroń T Juanes-Marcos JC Kasemo B Kroes GJ Ljubić I Naujoks N Nørskov JK Olsen RA Pendolino F Remhof A Románszki L Tekin A Vegge T Zäch M Züttel A 《Physical chemistry chemical physics : PCCP》2011,13(38):16955-16972
The widespread adoption of hydrogen as an energy carrier could bring significant benefits, but only if a number of currently intractable problems can be overcome. Not the least of these is the problem of storage, particularly when aimed at use onboard light-vehicles. The aim of this overview is to look in depth at a number of areas linked by the recently concluded HYDROGEN research network, representing an intentionally multi-faceted selection with the goal of advancing the field on a number of fronts simultaneously. For the general reader we provide a concise outline of the main approaches to storing hydrogen before moving on to detailed reviews of recent research in the solid chemical storage of hydrogen, and so provide an entry point for the interested reader on these diverse topics. The subjects covered include: the mechanisms of Ti catalysis in alanates; the kinetics of the borohydrides and the resulting limitations; novel transition metal catalysts for use with complex hydrides; less common borohydrides; protic-hydridic stores; metal ammines and novel approaches to nano-confined metal hydrides. 相似文献
84.
We call the digraph D an k-colored digraph if the arcs of D are colored with k colors. A subdigraph H of D is called monochromatic if all of its arcs are colored alike. A set N⊆V(D) is said to be a kernel by monochromatic paths if it satisfies the following two conditions: (i) for every pair of different vertices u,v∈N, there is no monochromatic directed path between them, and (ii) for every vertex x∈(V(D)?N), there is a vertex y∈N such that there is an xy-monochromatic directed path. In this paper, we prove that if D is an k-colored digraph that can be partitioned into two vertex-disjoint transitive tournaments such that every directed cycle of length 3,4 or 5 is monochromatic, then D has a kernel by monochromatic paths. This result gives a positive answer (for this family of digraphs) of the following question, which has motivated many results in monochromatic kernel theory: Is there a natural numberlsuch that if a digraphDisk-colored so that every directed cycle of length at mostlis monochromatic, thenDhas a kernel by monochromatic paths? 相似文献
85.
Abstract High—pressure crystal structure studies have been performed on Sm up to 100 GPa using synchrotron x-radiation and a diamond anvil cell. The structural sequence Sm-dhcp-fcc-dist.fcc has been confirmed. There is no evidence of any volume collapse. The bulk modulus and its pressure derivative have been determined (B0 = 30.7 GPa, B0’ = 2.5). 相似文献
86.
The VF3-type compounds MF3 with M = Fe and Ga have been studied by high-pressure energy-dispersive X-ray diffraction. The compression mechanism was found to be highly anisotropic for both compounds, with the c-axis showing little pressure dependence. The volume reduction is mainly achieved through coupled rotations of the MF6 octahedra around the c-axis, which reduces the length of the a-axis. The compression mechanism of both compounds is reasonably well described in terms of deformation of an 8/3/c2 sphere-packing model up to the pressures where the fluorine atoms become hexagonally close-packed. It is proposed that both compounds enter a phase with the fluorine atom arranged in a “super-dense” sphere packing at higher pressures. The zero pressure bulk modulus of FeF3 and GaF3 was determined as 12(2) and 37(3) GPa, respectively, and a scaling relation between the zero pressure bulk modulus and unit cell volumes was found for TiF3, CrF3, FeF3 and GaF3. 相似文献
87.
Abstract The high-pressure crystal structures of the compounds UX, where X = N, P, As and Sb, have been studied using X-ray diffraction in the pressure range up to about 60 GPa Rhornbohedral distortions are observed for UN and Up above 29 GPa and lO GPa, respectively. In Up a further transformation to an orthorhombic phase occurs at 28 GPa. UAs and USb transform to the CsCl structure at 20 GPa and 9 GPa, respectively. The latter transformations show a considerable hysteresis when the pressure is released. The scaling behaviour of the bulk modulus has been studied. It is confirmed that a log-log plot of bulk modulus versus specific volume for the cubic phases gives a straight line with a slope near ? 5/3. 相似文献
88.
This is a survey on geometric constructions in multifractal analysis of measures. We show that the multifractal formalism introduced by Olsen [Ol11] and Peyriére [Pey] leads to a multifractal geometry for product measures, for slices of measures (i.e. intersections of measures with lower dimensional subspaces), and for general intersections of measures, which is analogous to the fractal geometry for product sets, for slices of sets (i.e. intersections of sets with lower dimensional subspaces), and for general intersections of sets, respectively. 相似文献
89.
R. Baur A. Breskin R. Chechik A. Drees C. Jacob U. Faschingbauer P. Fischer Z. Fraenkel E. Gatti P. Glässel Th. Günzel C. P. de los Heros F. Hess D. Irmscher B. Lenkeit L. H. Olsen Y. Panebrattsev A. Pfeiffer I. Ravinovich P. Rehak A. Schön J. Schukraft J. Schukraft M. Sampietro A. Shor H. J. Specht V. Steiner S. Tapprogge G. Tel-Zur I. Tserruya Th. Ullrich J. P. Wurm 《Zeitschrift fur Physik C Particles and Fields》1997,74(4):593-594
90.
Four equidistant peaks are observed below the Kα1,2 line in the X-ray spectra of Na, Al, Si, SiO2, Ca, Sc and Ti, produced by oxygen bombardment. With much weaker intensity, these lines are also seen in proton excitation. The lines are interpreted to be due to the excitation of one or more volume plasmons in the target material by the Kα1,2 X-ray decay. 相似文献