962 resultados para metallosupramolecular architectures


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Two main perspectives have been developed within the Multidisciplinary Design Optimization (MDO) literature for classifying and comparing MDO architectures: a numerical point of view and a formulation/data flow point of view. Although significant work has been done here, these perspectives have not provided much in the way of a priori information or predictive power about architecture performance. In this report, we outline a new perspective, called the geometric perspective, which we believe will be able to provide such predictive power. Using tools from differential geometry, we take several prominent architectures and describe mathematically how each constructs the space through which it moves. We then consider how the architecture moves through the space which it has constructed. Taken together, these investigations show how each architecture relates to the original feasible design manifold, how the architectures relate to each other, and how each architecture deals with the design coupling inherent to the original system. This in turn lays the groundwork for further theoretical comparisons between and analyses of MDO architectures and their behaviour using tools and techniques derived from differential geometry. © 2012 by the American Institute of Aeronautics and Astronautics, Inc. All rights reserved.

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Single-electron devices (SEDs) have ultra-low power dissipation and high integration density, which make them promising candidates as basic circuit elements of the next generation VLSI circuits. In this paper, we propose two novel circuit single-electron architectures: the single-electron simulated annealing algorithm (SAA) circuit and the single-electron cellular neural network (CNN). We used the MOSFET-based single-electron turnstile [1] as the basic circuit element. The SAA circuit consists of the voltage-controlled single-electron random number generator [2] and the single-electron multiple-valued memories (SEMVs) [3]. The random-number generation and variable variations in SAA are easily achieved by transferring electrons using the single-electron turnstile. The CNN circuit used the floating-gate single-electron turnstile as the neural synapses, and the number of electrons is used to represent the cells states. These novel circuits are promising in future nanoscale integrated circuits.

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Rhombohedral-calcite and hexagonal-vaterite types of LuBO:Eu3+ microparticles with various complex self-assembled 3D architectures have been prepared selectively by an efficient surfactant- and template-free hydrothermal process for the first time. X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectrometry, transmission electron microscopy, high-resolution transmission electron microscopy, selected area electron diffraction, photoluminescence, and cathodoluminescence spectra as well as kinetic decays were used to characterize the samples.

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Strontium hydroxyapatite (Sr-5(PO4)(3)OH, SrHAp) microspheres with 3D architectures have been successfully prepared through a efficient and facile solvothermal process. The experimental results indicate that the SrHAP microspheres are composed of a large amount of nanosheets, which are assembled in a radial form from the center to the surface of the microspheres. The as-obtained SrHAp samples show an intense and bright blue emission from 350 to 570 nm centered at 427 nm (CIE coordinates: x = 0.153, y = 0.081; lifetime: 9.2 ns; quantum efficiency: 31%) under long-wavelength UV light excitation (344 nm). This blue emission might result from the CO2 center dot- radical impurities in the crystal lattice. Furthermore, the surfactants CTAB and trisodium citrate have an obvious impact on the morphologies and the luminescence properties of the products, respectively.

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The ordered-sphere CePO4 hierarchical architectures have been successfully synthesized by a simple hydrothermal method through the controlled growth of the CePO4 nanorods and self-assemble hierarchical structure under various reaction conditions. The evolution of the morphology of the samples has been investigated in detail. It was found that the coexistence of citric acid and cetaltrimethylammonium bromide in the reaction system plays an important role in the formation of the spherical CePO4 hierarchical architectures. A possible mechanism of the formation and growth of the hierarchical structure was suggested according to the experimental results and analysis. The effects of the reaction time as well as the variation of the morphologies on the luminescent properties of the products were also studied.

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Sheaflike terbium phosphate hydrate hierarchical architectures composed of filamentary nanorods have been fabricated by a hydrothermal method. The X-ray diffraction patterns and thermogravimetric/differential thermal analysis investigations reveal that the obtained terbium phosphate hydrate has a structural formula of TbPO4 center dot H2O, which can be readily indexed to the hexagonal phase GdPO4 center dot nH(2)O in JCPDS file 39-0232. The evolution of the morphology of the products has been investigated in detail. It is found that the addition of CTAB and Na2H2L (disodium ethylenediamine tetraacetate) plays an important role in controlling the final morphology of the products. A possible formation mechanism of the sheaflike architectures was proposed according to the experimental results and analysis. In addition, the phase structure of the product changes to monoclinic phase when it is annealed at 750 degrees C for 2 h in N-2-H-2 atmosphere. Tetragonal chase TbPO4 can be obtained when annealed temperature increases to 1150 degrees C.

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The large-scale synthesis of the metal-organic framework Eu(1,3,5-BTC)center dot 6H(2)O nanocrystallites with delicate morphologies such as sheaflike, butterflylike, and flowerlike superstructures composed of nanowires have been realized via a simple solution phase method at room temperature. Time-dependent experiments indicate that these superstructures were constructed by the splitting crystal growth mechanism, as has been noted in some minerals in nature. The synthetic parameters such as reaction time, concentration and molar ratio of reactants, surfactant, and reaction temperature all affected the morphology of the Eu(1,3,5-BTC)center dot 6H(2)O architectures. These well-arranged architectures exhibit red emission corresponding to the D-5(0) -> F-7(2) transition of the Eu3+ ions under UV light excitation, and the lifetime is determined to be about 0.22 ms.

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One mu-dichloro bridged diiridium complex and three mononuclear iridium(III) complexes based on the 1,3,4-oxadiazole derivatives as cyclometalated ligands and acetylacetonate (acac) or dithiolates O,O'-diethyldithiophosphate (Et(2)dtp) or N,N'-diethyldithiocarbamate (Et(2)dtc) as ancillary ligands have been synthesized and systematically studied by X-ray diffraction analysis. The results reveal that three mononuclear complexes all adopt distorted octahedral coordination geometry around the iridium center by two chelating ligands with cis-C-C and trans-N-N dispositions, which have the same coordination mode as the diiridium dimer. The dinuclear complex crystallizes in the monoclinic system and space group C2/c, whereas three mononuclear iridium complexes are all triclinic system and space group P(1) over bar. In the stacking structure of the dimer, one-dimensional tape-like chains along the b-axis are formed by hydrogen bondings, which are strengthened by pi stacking interactions between phenyl rings of 1,3,4-oxadiazole ligands. Then these chains assemble a three-dimensional alternating peak and valley fused wave-shape structure. In each stacking structure of three mononuclear complexes, two molecules form a dimer by the C-H center dot center dot center dot O hydrogen bondings, and these dimers are connected by pi stacking interactions along the b-axis, constructing a zigzag chain.

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Reaction of 2,6-pyridinedicarboxylic with CoCl2 . 6H(2)O in aqueous solution give rise to a three-dimensional Complex CO2(2,6-DPC)(2)Co(H2O)(5).2H(2)O (DPC = 2,6-pyridinedicarboxylate) 1. It has been characterized by elemental analyses, infrared spectra (IR) spectrum, thermogravimetric (TG) analysis, EPR spectrum, and single crystal X-ray diffraction. The complex crystallizes in the P2(1)/c space group with a = 8.3906(3) Angstrom, b = 27.4005(8) Angstrom, c = 9.6192(4) A, alpha = 90.00degrees, beta = 98.327(2)degrees, gamma = 90.00degrees, V = 2188.20(14) Angstrom(3), Z = 4. There are two types of cobalt environments: Co(1) is coordinated by four oxygen atoms from four carboxyl groups and two nitrogen 2 atoms which are all from pdc(2). Co(2) is coordinated by six oxygen atoms, five from coordinated water molecules and one from a carboxyl of pdc(2) - of which the other oxygen atom is linked to the Co(1). The extensive intermolecular hydrogen bonds are formed in the crystal by means of the five coordinated water molecules.

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The Expectation-Maximization (EM) algorithm is an iterative approach to maximum likelihood parameter estimation. Jordan and Jacobs (1993) recently proposed an EM algorithm for the mixture of experts architecture of Jacobs, Jordan, Nowlan and Hinton (1991) and the hierarchical mixture of experts architecture of Jordan and Jacobs (1992). They showed empirically that the EM algorithm for these architectures yields significantly faster convergence than gradient ascent. In the current paper we provide a theoretical analysis of this algorithm. We show that the algorithm can be regarded as a variable metric algorithm with its searching direction having a positive projection on the gradient of the log likelihood. We also analyze the convergence of the algorithm and provide an explicit expression for the convergence rate. In addition, we describe an acceleration technique that yields a significant speedup in simulation experiments.

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We consider a Delay Tolerant Network (DTN) whose users (nodes) are connected by an underlying Mobile Ad hoc Network (MANET) substrate. Users can declaratively express high-level policy constraints on how “content” should be routed. For example, content can be directed through an intermediary DTN node for the purposes of preprocessing, authentication, etc., or content from a malicious MANET node can be dropped. To support such content routing at the DTN level, we implement Predicate Routing [1] where high-level constraints of DTN nodes are mapped into low-level routing predicates within the MANET nodes. Our testbed [2] uses a Linux system architecture with User Mode Linux [3] to emulate every DTN node with a DTN Reference Implementation code [4]. In our initial architecture prototype, we use the On Demand Distance Vector (AODV) routing protocol at the MANET level. We use the network simulator ns-2 (ns-emulation version) to simulate the wireless connectivity of both DTN and MANET nodes. Preliminary results show the efficient and correct operation of propagating routing predicates. For the application of content re-routing through an intermediary, as a side effect, results demonstrate the performance benefit of content re-routing that dynamically (on-demand) breaks the underlying end-to-end TCP connections into shorter-length TCP connections.

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To construct high performance Web servers, system builders are increasingly turning to distributed designs. An important challenge that arises in distributed Web servers is the need to direct incoming connections to individual hosts. Previous methods for connection routing have employed a centralized node which handles all incoming requests. In contrast, we propose a distributed approach, called Distributed Packet Rewriting (DPR), in which all hosts of the distributed system participate in connection routing. We argue that this approach promises better scalability and fault-tolerance than the centralized approach. We describe our implementation of four variants of DPR and compare their performance. We show that DPR provides performance comparable to centralized alternatives, measured in terms of throughput and delay under the SPECweb96 benchmark. Finally, we argue that DPR is particularly attractive both for small scale systems and for systems following the emerging trend toward increasingly intelligent I/O subsystems.

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The recognition of 3-D objects from sequences of their 2-D views is modeled by a family of self-organizing neural architectures, called VIEWNET, that use View Information Encoded With NETworks. VIEWNET incorporates a preprocessor that generates a compressed but 2-D invariant representation of an image, a supervised incremental learning system that classifies the preprocessed representations into 2-D view categories whose outputs arc combined into 3-D invariant object categories, and a working memory that makes a 3-D object prediction by accumulating evidence from 3-D object category nodes as multiple 2-D views are experienced. The simplest VIEWNET achieves high recognition scores without the need to explicitly code the temporal order of 2-D views in working memory. Working memories are also discussed that save memory resources by implicitly coding temporal order in terms of the relative activity of 2-D view category nodes, rather than as explicit 2-D view transitions. Variants of the VIEWNET architecture may also be used for scene understanding by using a preprocessor and classifier that can determine both What objects are in a scene and Where they are located. The present VIEWNET preprocessor includes the CORT-X 2 filter, which discounts the illuminant, regularizes and completes figural boundaries, and suppresses image noise. This boundary segmentation is rendered invariant under 2-D translation, rotation, and dilation by use of a log-polar transform. The invariant spectra undergo Gaussian coarse coding to further reduce noise and 3-D foreshortening effects, and to increase generalization. These compressed codes are input into the classifier, a supervised learning system based on the fuzzy ARTMAP algorithm. Fuzzy ARTMAP learns 2-D view categories that are invariant under 2-D image translation, rotation, and dilation as well as 3-D image transformations that do not cause a predictive error. Evidence from sequence of 2-D view categories converges at 3-D object nodes that generate a response invariant under changes of 2-D view. These 3-D object nodes input to a working memory that accumulates evidence over time to improve object recognition. ln the simplest working memory, each occurrence (nonoccurrence) of a 2-D view category increases (decreases) the corresponding node's activity in working memory. The maximally active node is used to predict the 3-D object. Recognition is studied with noisy and clean image using slow and fast learning. Slow learning at the fuzzy ARTMAP map field is adapted to learn the conditional probability of the 3-D object given the selected 2-D view category. VIEWNET is demonstrated on an MIT Lincoln Laboratory database of l28x128 2-D views of aircraft with and without additive noise. A recognition rate of up to 90% is achieved with one 2-D view and of up to 98.5% correct with three 2-D views. The properties of 2-D view and 3-D object category nodes are compared with those of cells in monkey inferotemporal cortex.