1,138 research outputs found

    Phase diagram of YBa2_2Cu3_3O7−y_{7-y} at T<<Tc_c based on Cu(2) transverse nuclear relaxation

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    Two maxima in transverse relaxation rate of Cu(2) nuclei in YBa2_2Cu3_3O7−y_{7-y} are observed, at T = 35 K and T = 47 K. Comparison of the 63^{63}Cu(2) and 65^{65}Cu(2) rates at T = 47 K indicates the magnetic character of relaxation. The enhancement at T = 47 K of fluctuating local magnetic fields perpendicular to the CuO2_2 planes is connected with the critical fluctuations of orbital currents. Maximum at T = 35 K is connected with the appearance of inhomogeneous supeconducting phase. Together with data published to date, our experimental results allow to suggest a qualitatively new phase diagram of the superconducting phase.Comment: 4 LaTEX pages + 3 figures in *.ps forma

    Autonomic Role and Mission Allocation Framework for Wireless Sensor Networks.

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    Pervasive applications incorporate physical components that are exposed to everyday use and a large number of conditions and external factors that can lead to faults and failures. It is also possible that application requirements change during deployment and the network needs to adapt to a new context. Consequently, pervasive systems must be capable to autonomically adapt to changing conditions without involving users becoming a transparent asset in the environment. In this paper, we present an autonomic mechanism for initial task assignment in sensor networks, an NP-hard problem. We also study on-line adaptation of the original deployment which considers real-time metrics for maximising utility and lifetime of applications and smooth service degradation in the face of component failures. © 2011 IEEE

    On the gas storage properties of 3D porous carbons derived from hyper-crosslinked polymers

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    The preparation of porous carbons by post-synthesis treatment of hypercrosslinked polymers is described, with a careful physico-chemical characterization, to obtain new materials for gas storage and separation. Different procedures, based on chemical and thermal activations, are considered; they include thermal treatment at 380 degrees C, and chemical activation with KOH followed by thermal treatment at 750 or 800 degrees C; the resulting materials are carefully characterized in their structural and textural properties. The thermal treatment at temperature below decomposition (380 degrees C) maintains the polymer structure, removing the side-products of the polymerization entrapped in the pores and improving the textural properties. On the other hand, the carbonization leads to a different material, enhancing both surface area and total pore volumethe textural properties of the final porous carbons are affected by the activation procedure and by the starting polymer. Different chemical activation methods and temperatures lead to different carbons with BET surface area ranging between 2318 and 2975 m(2)/g and pore volume up to 1.30 cc/g. The wise choice of the carbonization treatment allows the final textural properties to be finely tuned by increasing either the narrow pore fraction or the micro- and mesoporous volume. High pressure gas adsorption measurements of methane, hydrogen, and carbon dioxide of the most promising material are investigated, and the storage capacity for methane is measured and discussed

    Water diffusion modulates the cest effect on Tb(III)-mesoporous silica probes

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    The anchoring of lanthanide(III) chelates on the surface of mesoporous silica nanoparticles (MSNs) allowed their investigation as magnetic resonance imaging (MRI) and chemical exchange saturation transfer (CEST) contrast agents. Since their efficiency is strongly related to the interaction occurring between Ln-chelates and \u201cbulk\u201d water, an estimation of the water diffusion inside MSNs channels is very relevant. Herein, a method based on the exploitation of the CEST properties of TbDO3A-MSNs was applied to evaluate the effect of water diffusion inside MSN channels. Two MSNs, namely MCM-41 and SBA-15, with different pores size distributions were functionalized with TbDO3A-like chelates and polyethylene glycol (PEG) molecules and characterized by HR-TEM microscopy, IR spectroscopy, N2 physisorption, and thermogravimetric analysis (TGA). The different distribution of Tb-complexes in the two systems, mainly on the external surface in case of MCM-41 or inside the internal pores for SBA-15, resulted in variable CEST efficiency. Since water molecules diffuse slowly inside silica channels, the CEST effect of the LnDO3A-SBA-15 system was found to be one order of magnitude lower than in the case of TbDO3A-MCM-41. The latter system reaches an excellent sensitivity of ca. 55 \ub1 5 \ub5M, which is useful for future theranostic or imaging applications

    GdDOTAGA(C18)2: an efficient amphiphilic Gd(iii) chelate for the preparation of self-assembled high relaxivity MRI nanoprobes

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    A new amphiphilic GdDOTA-like complex functionalized with two octadecyl chains was synthesised and incorporated into the bilayer of liposomes and dendrimersomes. (1)H NMR relaxometric studies and in vivo MRI experiments on mice bearing a syngeneic melanoma tumour have shown a great improvement in performance

    Surprising Complexity of the [Gd(AAZTA)(H2O)2]- Chelate Revealed by NMR in the Frequency and Time Domains

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    Typically, Ln(III) complexes are isostructural along the series, which enables studying one particular metal chelate to derive the structural features of the others. This is not the case for [Ln(AAZTA)(H2O)x]- (x = 1, 2) systems, where structural variations along the series cause changes in the hydration number of the different metal complexes, and in particular the loss of one of the two metal-coordinated water molecules between Ho and Er. Herein, we present a 1H field-cycling relaxometry and 17O NMR study that enables accessing the different exchange dynamics processes involving the two water molecules bound to the metal center in the [Gd(AAZTA)(H2O)2]- complex. The resulting picture shows one Gd-bound water molecule with an exchange rate ∼6 times faster than that of the other, due to a longer metal-water distance, in accordance with density functional theory (DFT) calculations. The substitution of the more labile water molecule with a fluoride anion in a diamagnetic-isostructural analogue of the Gd-complex, [Y(AAZTA)(H2O)2]-, allows us to follow the chemical exchange process by high-resolution NMR and to describe its thermodynamic behavior. Taken together, the variety of tools offered by NMR (including high-resolution 1H, 19F NMR as a function of temperature, 1H longitudinal relaxation rates vs B0, and 17O transverse relaxation rates vs T) provides a complete description of the structure and exchange dynamics of these Ln-complexes along the series

    Rigid and Compact Binuclear Bis-hydrated Gd-complexes as High Relaxivity MRI Agents

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    The first binuclear Gd-complex of the 12-membered pyridine-based polyaminocarboxylate macrocyclic ligand PCTA was synthesized by C−C connection of the pyridine units through two different synthetic procedures. A dimeric AAZTA-ligand was also synthesized with the aim to compare the relaxometric results or the two ditopic Gd-complexes. Thus, the 1H relaxometric study on [Gd2PCTA2(H2O)4] and on [Gd2AAZTA2(H2O)4]2− highlighted the remarkable rigidity and compactness of the two binuclear complexes, which results in molar relaxivities (per Gd), at 1.5 T and 298 K of ca. 12–12.6 mM−1 s−1 with an increase of ca. 80 % at 1.5 T and 298 K (+70 % at 310 K) with respect to the corresponding mononuclear complexes

    Thermodynamic and Kinetic Stabilities of Al(III) Complexes with N2O3 Pentadentate Ligands

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    : Al(III) complexes have been recently investigated for their potential use in imaging with positron emission tomography (PET) by formation of ternary complexes with the radioisotope fluorine-18 (18F). Although the derivatives of 1,4,7-triazacyclononane-1,4,7-triacetic acid (NOTA) are the most applied chelators for [Al18F]2+ labelling and (pre)clinical PET imaging, non-macrocyclic, semi-rigid pentadentate chelators having two N- and three O-donor atoms such as RESCA1 and AMPDA-HB have been proposed with the aim to allow room temperature labelling of temperature-sensitive biomolecules. The paucity of stability data on Al(III) complexes used for PET imaging instigated a complete thermodynamic and kinetic solution study on Al(III) complexes with aminomethylpiperidine (AMP) derivatives AMPTA and AMPDA-HB and the comparison with a RESCA1-like chelator CD3A-Bn (trans-1,2-diaminocyclohexane-N-benzyl-N,N',N'-triacetic acid). The stability constant of [Al(AMPDA-HB)] is about four orders of magnitude higher than that of [Al(AMPTA)] and [Al(CD3A-Bn)], highlighting the greater affinity of phenolates with respect to acetate O-donors. On the other hand, the kinetic inertness of the complexes, determined by following the Cu2+-mediated transmetallation reactions in the 7.5-10.5 pH range, resulted in a spontaneous and hydroxide-assisted dissociation slightly faster for [Al(AMPTA)] than for the other two complexes (t1/2 = 4.5 h for [Al(AMPTA)], 12.4 h for [Al(AMPDA-HB)], and 24.1 h for [Al(CD3A-Bn)] at pH 7.4 and 25 °C). Finally, the [AlF]2+ ternary complexes were prepared and their stability in reconstituted human serum was determined by 19F NMR experiments

    Energy-Aware Network-on-Chip Application Mapping Based on Domain Knowledge Genetic Algorithm

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    This paper addresses energy-aware application mapping for large-scale Network-on-chip (NoC). The increasing number of intellectual property (IP) cores in multi-processor system-on-chips (MPSoCs) makes NoC application mapping more challenging to find optimum core-to-topology mapping. This paper proposes an application mapping technique that incorporates domain knowledge into genetic algorithm (GA) to minimize the energy consumption of NoC communication. The GA is initialized with knowledge on network partition whereas the genetic crossover operator is guided with inter-core communication demands. NoC energy estimation is based on analytical energy model and cycle-accurate Noxim simulation. For large-scale NoC, application mapping using knowledge-based genetic operator saves up to 28% energy compared to the one on conventional GA. Adding knowledge-based initial mapping speeds up convergence by 81% and further saves energy by 5% compared to only knowledge-based crossover GA. Furthermore, cycle-accurate simulations of applications with traffic dependency show the effectiveness of the proposed application mapping for large-scale NoC
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