2,223 research outputs found

    Crystallography, magnetic susceptibility, heat capacity, and electrical resistivity of heavy fermion LiV2_2O4_4 single crystals grown using a self-flux technique

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    Magnetically pure spinel compound LiV2O4{\rm LiV_2O_4} is a rare dd-electron heavy fermion. Measurements on single crystals are needed to clarify the mechanism for the heavy fermion behavior in the pure material. In addition, it is known that small concentrations (<1< 1 mol%) of magnetic defects in the structure strongly affect the properties, and measurements on single crystals containing magnetic defects would help to understand the latter behaviors. Herein, we report flux growth of LiV2O4{\rm LiV_2O_4} and preliminary measurements to help resolve these questions. The magnetic susceptibility of some as-grown crystals show a Curie-like upturn at low temperatures, showing the presence of magnetic defects within the spinel structure. The magnetic defects could be removed in some of the crystals by annealing them at 700 ^\circC\@. A very high specific heat coefficient γ\gamma = 450 mJ/(mol K2{^2}\@) was obtained at a temperature of 1.8 K for a crystal containing a magnetic defect concentration nndefect{\rm_{defect}} = 0.5 mol%. A crystal with nndefect{\rm _{defect}} = 0.01 mol% showed a residual resistivity ratio of 50.Comment: 6 pages, 7 figures, Title modifie

    The reductive activation of CO2 across a Ti═Ti double bond: synthetic, structural, and mechanistic studies

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    [Image: see text] The reactivity of the bis(pentalene)dititanium double-sandwich compound Ti(2)Pn(†)(2) (1) (Pn(†) = 1,4-{Si(i)Pr(3)}(2)C(8)H(4)) with CO(2) is investigated in detail using spectroscopic, X-ray crystallographic, and computational studies. When the CO(2) reaction is performed at −78 °C, the 1:1 adduct 4 is formed, and low-temperature spectroscopic measurements are consistent with a CO(2) molecule bound symmetrically to the two Ti centers in a μ:η(2),η(2) binding mode, a structure also indicated by theory. Upon warming to room temperature the coordinated CO(2) is quantitatively reduced over a period of minutes to give the bis(oxo)-bridged dimer 2 and the dicarbonyl complex 3. In situ NMR studies indicated that this decomposition proceeds in a stepwise process via monooxo (5) and monocarbonyl (7) double-sandwich complexes, which have been independently synthesized and structurally characterized. 5 is thermally unstable with respect to a μ-O dimer in which the Ti–Ti bond has been cleaved and one pentalene ligand binds in an η(8) fashion to each of the formally Ti(III) centers. The molecular structure of 7 shows a “side-on” bound carbonyl ligand. Bonding of the double-sandwich species Ti(2)Pn(2) (Pn = C(8)H(6)) to other fragments has been investigated by density functional theory calculations and fragment analysis, providing insight into the CO(2) reaction pathway consistent with the experimentally observed intermediates. A key step in the proposed mechanism is disproportionation of a mono(oxo) di-Ti(III) species to yield di-Ti(II) and di-Ti(IV) products. 1 forms a structurally characterized, thermally stable CS(2) adduct 8 that shows symmetrical binding to the Ti(2) unit and supports the formulation of 4. The reaction of 1 with COS forms a thermally unstable complex 9 that undergoes scission to give mono(μ-S) mono(CO) species 10. Ph(3)PS is an effective sulfur transfer agent for 1, enabling the synthesis of mono(μ-S) complex 11 with a double-sandwich structure and bis(μ-S) dimer 12 in which the Ti–Ti bond has been cleaved

    Implicit learning of affective responses in dementia patients: a face-emotion-association paradigm

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    The aim of the present study was to develop and evaluate an ecologically valid approach to assess implicit learning of affective responses in dementia patients. We designed a Face-Emotion-Association paradigm (FEA) that allows to quantify the influence of stimuli with positive and negative valence on affective responses. Two pictures of neutral male faces are rated on the dimensions of valence and arousal before and after aversive versus pleasant fictitious biographical information is paired with each of the pictures. At the second measurement time point, memory for pictures and biographical content is tested. The FEA was tested in 21 patients with dementia and 13 healthy controls. Despite severely impaired explicit memory, patients changed valence and arousal ratings according to the biographical content and did not differ in their ratings from the control group. The results demonstrate that our FEA paradigm is a valid instrument to investigate learning of affective responses in dementia patients

    Epidermal Growth Factor–PEG Functionalized PAMAM-Pentaethylenehexamine Dendron for Targeted Gene Delivery Produced by Click Chemistry

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    Aim of this study was the site-specific conjugation of an epidermal growth factor (EGF)-polyethylene glycol (PEG) chain by click chemistry onto a poly(amido amine) (PAMAM) dendron, as a key step toward defined multifunctional carriers for targeted gene delivery. For this purpose, at first propargyl amine cored PAMAM dendrons with ester ends were synthesized. The chain terminal ester groups were then modified by oligoamines with different secondary amino densities. The oligoamine-modified PAMAM dendrons were well biocompatible, as demonstrated in cytotoxicity assays. Among the different oligoamine-modified dendrons, PAMAM-pentaethylenehexamine (PEHA) dendron polyplexes displayed the best gene transfer ability. Conjugation of PAMAM-PEHA dendron with PEG spacer was conducted via click reaction, which was performed before amidation with PEHA. The resultant PEG-PAMAM-PEHA copolymer was then coupled with EGF ligand. pDNA transfections in HuH-7 hepatocellular carcinoma cells showed a 10-fold higher efficiency with the polyplexes containing conjugated EGF as compared to the ligand-free ones, demonstrating the concept of ligand targeting. Overall gene transfer efficiencies, however, were moderate, suggesting that additional measures for overcoming subsequent intracellular bottlenecks in delivery have to be taken

    Testing variational estimation of process parameters and initial conditions of an earth system model

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    We present a variational assimilation system around a coarse resolution Earth System Model (ESM) and apply it for estimating initial conditions and parameters of the model. The system is based on derivative information that is efficiently provided by the ESM's adjoint, which has been generated through automatic differentiation of the model's source code. In our variational approach, the length of the feasible assimilation window is limited by the size of the domain in control space over which the approximation by the derivative is valid. This validity domain is reduced by non-smooth process representations. We show that in this respect the ocean component is less critical than the atmospheric component. We demonstrate how the feasible assimilation window can be extended to several weeks by modifying the implementation of specific process representations and by switching off processes such as precipitation

    Search for W~1Z~2\widetilde{W}_1\widetilde{Z}_2 Production via Trilepton Final States in ppˉp\bar{p} collisions at s=1.8\sqrt{s}=1.8 TeV

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    We have searched for associated production of the lightest chargino, W~1\widetilde{W}_1, and next-to-lightest neutralino, Z~2\widetilde{Z}_2, of the Minimal Supersymmetric Standard Model in ppˉp\bar{p} collisions at \mbox{s\sqrt{s} = 1.8 TeV} using the \D0 detector at the Fermilab Tevatron collider. Data corresponding to an integrated luminosity of 12.5±0.7\pm 0.7 \ipb were examined for events containing three isolated leptons. No evidence for W~1Z~2\widetilde{W}_1\widetilde{Z}_2 pair production was found. Limits on σ(W~1Z~2)\sigma(\widetilde{W}_1\widetilde{Z}_2)Br(W~1lνZ~1)(\widetilde{W}_1\to l\nu\widetilde{Z}_1)Br(Z~2llˉZ~1)(\widetilde{Z}_2\to l\bar{l}\widetilde{Z}_1) are presented.Comment: 17 pages (13 + 1 page table + 3 pages figures). 3 PostScript figures will follow in a UUEncoded, gzip'd, tar file. Text in LaTex format. Submitted to Physical Review Letters. Replace comments - Had to resumbmit version with EPSF directive

    The African Political Business Cycle: Varieties of Experience

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    We seek to understand both the incidence and the impact of the African political business cycle in the light of a literature which has argued that, with major extensions of democracy since the 1990s, the cycle has both become more intense and has made African political systems more fragile. With the help of country-case studies, we argue, first, that the African political business cycle is not homogeneous, and occurs relatively infrequently in so-called ‘dominant-party systems’ where a pre-election stimulus confers little political advantage. Secondly, we show that, in those countries where a political cycle does occur, it does not necessarily cause institutional damage. Whether it does or not depends not so much on whether there is an electoral cycle as on whether this cycle calms or exacerbates fears of an unjust allocation of resources. In other words, the composition of the pre-election stimulus, in terms of its allocation between different categories of voter, is as important as its size

    Probing BFKL Dynamics in the Dijet Cross Section at Large Rapidity Intervals in ppbar Collisions at sqrt{s}=1800 and 630 GeV

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    Inclusive dijet production at large pseudorapidity intervals (delta_eta) between the two jets has been suggested as a regime for observing BFKL dynamics. We have measured the dijet cross section for large delta_eta in ppbar collisions at sqrt{s}=1800 and 630 GeV using the DO detector. The partonic cross section increases strongly with the size of delta_eta. The observed growth is even stronger than expected on the basis of BFKL resummation in the leading logarithmic approximation. The growth of the partonic cross section can be accommodated with an effective BFKL intercept of a_{BFKL}(20GeV)=1.65+/-0.07.Comment: Published in Physical Review Letter

    Search for R-parity Violating Supersymmetry in Dimuon and Four-Jets Channel

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    We present results of a search for R-parity-violating decay of the neutralino chi_1^0, taken to be the Lightest Supersymmetric Particle. It is assumed that this decay proceeds through one of the lepton-number violating couplings lambda-prime_2jk (j=1,2; k=1,2,3). This search is based on 77.5 pb-1 of data, collected by the D0 experiment at the Fermilab Tevatron in ppbar collisions at a center of mass energy of 1.8 TeV in 1992-1995.Comment: 10 pages, 3 figure

    Differential Production Cross Section of Z Bosons as a Function of Transverse Momentum at sqrt{s}=1.8 TeV

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    We present a measurement of the transverse momentum distribution of Z bosons produced in ppbar collisions at sqrt{s}=1.8 TeV using data collected by the D0 experiment at the Fermilab Tevatron Collider during 1994--1996. We find good agreement between our data and a current resummation calculation. We also use our data to extract values of the non-perturbative parameters for a particular version of the resummation formalism, obtaining significantly more precise values than previous determinations.Comment: 10 pages, 2 figures, submitted to Phys. Rev. Letters v2 has margin error correcte
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