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21.
Dr. S. James Ratnakar Dr. Sara Chirayil Dr. Alexander M. Funk Dr. Shanrong Zhang Prof. João F. Queiró Prof. Carlos F. G. C. Geraldes Prof. Zoltan Kovacs Prof. A. Dean Sherry 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(48):21855-21860
Paramagnetic chemical exchange saturation transfer (paraCEST) agents are well-suited for imaging tissue pH because the basis of CEST, chemical exchange, is inherently sensitive to pH. Several previous pH-sensitive paraCEST agents were based on an exchanging Ln3+-bound water molecule as the CEST antenna but this design often added additional line-broadening to the bulk water signal due to T2 exchange. We report herein a pH-sensitive paraCEST agent that lacks an inner-sphere water molecule but contains one Ln-bound −OH group for CEST activation. The Yb3+ complex, Yb( 1 ), displayed a single, highly shifted CEST peak originating from the exchangeable Yb-OH proton, the frequency of which changed over the biologically relevant pH range. CEST images of phantoms ranging in pH from 6 to 8 demonstrate the potential of this agent for imaging pH. Initial rodent imaging studies showed that Gd( 1 ) remains in the vascular system much longer than anticipated but is cleared slowly via renal filtration. 相似文献
22.
I. P. Studenyak M. Kranjcec L. M. Suslikov D. Sh. Kovacs V. V. Pan’ko 《Optics and Spectroscopy》2002,92(4):532-535
The absorption edge in Cu6P(S1?x Sex)5Br crystals has been studied for strong absorption in the temperature range of 77–330 K. The parameters of the Urbach absorption edge and exciton-phonon interactions in Cu6P(S1-x Sex)5Br crystals are determined and their effect on the composition disorder is studied. 相似文献
23.
24.
A. J. Kovacs J. J. Aklonis J. M. Hutchinson A. R. Ramos 《Journal of Polymer Science.Polymer Physics》1979,17(7):1097-1162
A multiordering parameter model for glass-transition phenomena has been developed on the basis of nonequilibrium thermodynamics. In this treatment the state of the glass is determined by the values of N ordering parameters in addition to T and P; the departure from equilibrium is partitioned among the various ordering parameters, each of which is associated with a unique retardation time. These times are assumed to depend on T, P, and on the instantaneous state of the system characterized by its overall departure from equilibrium, giving rise to the well-known nonlinear effects observed in volume and enthalpy recovery. The contribution of each ordering parameter to the departure and the associated retardation times define the fundamental distribution function (the structural retardation spectrum) of the system or, equivalently, its fundamental material response function. These, together with a few experimentally measurable material constants, completely define the recovery behavior of the system when subjected to any thermal treatment. The behavior of the model is explored for various classes of thermal histories of increasing complexity, in order to simulate real experimental situations. The relevant calculations are based on a discrete retardation spectrum, extending over four time decades, and on reasonable values of the relevant material constants in order to imitate the behavior of polymer glasses. The model clearly separates the contribution of the retardation spectrum from the temperature-structure dependence of the retardation times which controls its shifts along the experimental time scale. This is achieved by using the natural time scale of the system which eliminates all the nonlinear effects, thus reducing the response function to the Boltzmann superposition equation, similar to that encountered in the linear viscoelasticity. As a consequence, the system obeys a rate (time) -temperature reduction rule which provides for generalization within each class of thermal treatment. Thus the model establishes a rational basis for comparing theory with experiment, and also various kinds of experiments between themselves. The analysis further predicts interesting features, some of which have often been overlooked. Among these are the impossibility of extraction of the spectrum (or response function) from experiments involving cooling from high temperatures at finite rate; and the appearance of two peaks in the expansion coefficient, or heat capacity, during the heating stage of three-step thermal cycles starting at high temperatures. Finally, the theory also provides a rationale for interpreting the time dependence of mechanical or other structure-sensitive properties of glasses as well as for predicting their long-range behavior. 相似文献
25.
Thermal behavior of glasses, as observed from the isobaric variations of volume, v, and enthalpy, H, is analyzed in terms of retardation kinetics. A phenomenological theory involving a single retardation time, τ, is developed, assuming that molecular mobility is controlled essentially by the actual free volume, or configurational entropy of the glassy specimen. The characteristic features of the v and H isobars, as derived from the theory, are examined as a function of the thermal history of a typical glassy specimen. The respective contributions of temperature and structural parameters to τ, are also discussed in terms of the characteristic parameters of the isobars. The theoretical predictions are compared with some dilatometric data obtained with an atactic polystyrene. The comparison reveals the limitations of the theoretical treatment and suggests that glass-transition phenomena involve more than one retardation mechanism. 相似文献
26.
Van Parijs SM Corkeron PJ Harvey J Hayes SA Mellinger DK Rouget PA Thompson PM Wahlberg M Kovacs KM 《The Journal of the Acoustical Society of America》2003,113(6):3403-3410
Comparative analyses of the roar vocalization of male harbor seals from ten sites throughout their distribution showed that vocal variation occurs at the oceanic, regional, population, and subpopulation level. Genetic barriers based on the physical distance between harbor seal populations present a likely explanation for some of the observed vocal variation. However, site-specific vocal variations were present between genetically mixed subpopulations in California. A tree-based classification analysis grouped Scottish populations together with eastern Pacific sites, rather than amongst Atlantic sites as would be expected if variation was based purely on genetics. Lastly, within the classification tree no individual vocal parameter was consistently responsible for consecutive splits between geographic sites. Combined, these factors suggest that site-specific variation influences the development of vocal structure in harbor seals and these factors may provide evidence for the occurrence of vocal dialects. 相似文献
27.
Barta C Ronai Z Nemoda Z Szekely A Kovacs E Sasvari-Szekely M Guttman A 《Journal of chromatography. A》2001,924(1-2):285-290
A microfabricated electrophoresis device was used for rapid polymerase chain reaction product analysis in genotyping the dopamine D4 receptor gene (DRD4) 48 base pairs repeat polymorphism. An allelic ladder, prepared from homozygous individuals, was used as internal standard during the microchip electrophoresis based analysis. Comparison of this novel separation method with the conventional slab gel and previously reported ultra-thin-layer techniques confirmed the reliability of this new method. Genotyping of 332 healthy Hungarian individuals gave the following allele frequencies: two-repeat: 0.089; three-repeat: 0.026; four-repeat: 0.674; five-repeat: 0.011; six-repeat: 0.002; seven-repeat: 0.189; eight-repeat: 0.011. The genotype frequencies obtained showed no deviation from the Hardy-Weinberg equilibrium (p>0.903), further underlying the reliability of this new genotyping technique. 相似文献
28.
P. Astier G. Bernardi G. Carugno J. Chauveau P. Chrysicopoulou J. Dumarchez M. Ferro-Luzzi F. Kovacs A. Letessier-Selvon J. -M. Levy M. J. Murtagh J. -M. Perreau Y. Pons J. L. Stone A. -M. Touchard F. Vannucci P. Wanderer D. H. White 《Physics letters. [Part B]》1989,220(4):646-652
A search for νμ→νe and
oscillations has been conducted with the AGS wide-band neutrino beam at the Brookhaven National Laboratory. We find more νe (
e) interactions than were expected on the basis of the number of incident νe (
e) calculated as part of the neutrino beam. The excess is about a factor two over the expectation, the statistical significance being about two and a half standard deviations for νe and weaker for
e. 相似文献
29.
György Bázár Zoltan Kovacs Mariko Tanaka Akane Furukawa Airi Nagai Manami Osawa Yukari Itakura Hiroshi Sugiyama Roumiana Tsenkova 《Analytica chimica acta》2015
Near infrared spectroscopy is an overtone spectroscopy regarded as a quick and non-destructive method that provides analytical solutions for components that represent approximately 1% or more of the total mass of the investigated composite samples. Aquaphotomics offers the possibility for disentanglement of information remaining hidden in the spectra when conventional data evaluation methods are used, since this concept utilizes changes of the water structure induced by the measured solute as specific molecular vibrations at water bands. Here, near infrared technique and aquaphotomics are applied for non-destructive identification and quantification of mono- and di-saccharide solutes at 100–0.02 mM concentration that is accepted as unachievable with near infrared spectroscopy. The results presented in this study support the aquaphotomics' water molecular mirror concept that explores spectral changes related to water molecular rearrangements caused by minute changes of the solutes in the aqueous systems. The method provides quick and accurate alternative for classical analytical measurements of saccharides even at millimolar concentration levels. 相似文献
30.
L. S. Khaikin O. E. Grikina G. V. Girichev A. Kovacs K. P. Dyugaev A. M. Astachov 《Russian Journal of Physical Chemistry A, Focus on Chemistry》2011,85(3):441-446
The structures and force fields of the equilibrium forms of 2-nitroguanidine (1), 1,1,3,3-tetramethyl-2-nitroguanidine (2), and nitroguanyl azide (3) were determined in the MP2(full)/6-311G(3df, 2p) approximation; wagging-inversion motions of the N amine atoms were studied. The internal rotation potential function of
the NO2 group was calculated for 1. Similar functions for 1 and 2 were also obtained in the MP2(full)/6-311G(d, p) approximation. Direct one-dimensional problems for a nonrigid model were solved by the variational method, and the distribution
of torsional levels was obtained. In the region of potential minimum, rotation in both molecules had the character of large-amplitude
motions. For the first time, electron diffractions data were obtained at 100°C for molecule 2 without noticeable traces of substance decomposition. A structural r
e
analysis was performed using the model of large-amplitude motions for characteristic NO2 group torsional vibrations. Vibrational corrections to internuclear distances and mean amplitudes were calculated taking
into account nonlinear kinematic effects using the force fields obtained in this work. The geometry of molecule 2 calculated in the MP2(full)/6-311G(3df, 2p) approximation well corresponds to the gas electron diffraction data. The parameters of molecule 2 in the crystalline phase, however, differ substantially from the parameters of the free molecule. This corresponds with the
suggestion of the influence of intermolecular H-bonds involving the imine nitrogen atom and nitro groups oxygen atoms. 相似文献