405 research outputs found

    ESR evidence for disordered magnetic phase from ultra-small carbon nanotubes embedded in zeolite nanochannels

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    A multi-frequency electron spin resonance (ESR) study provides evidence for the occurrence of low temperature ferromagnetic/spin-glass behavior in aligned arrays of sub-nanometer single walled carbon nanotubes confined in zeolite nano-channels, owing to sp2-type non-bonding carbon associated localized states with density of ~3 x 1019 /g. Features related to the much anticipated conduction ESR are not detected. In the paramagnetic phase, the ESR linewidth is found to be weakly dependent on microwave frequency.Comment: Accepted to be published in EuroPhysics Letter

    Semiclassical bounds on dynamics of two-dimensional interacting disordered fermions

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    Using the truncated Wigner approximation (TWA) we study quench dynamics of two-dimensional lattice systems consisting of interacting spinless fermions with potential disorder. First, we demonstrate that the semiclassical dynamics generally relaxes faster than the full quantum dynamics. We obtain this result by comparing the semiclassical dynamics with exact diagonalization and Lanczos propagation of one-dimensional chains. Next, exploiting the TWA capabilities of simulating large lattices, we investigate how the relaxation rates depend on the dimensionality of the studied system. We show that strongly disordered one-dimensional and two-dimensional systems exhibit a transient, logarithmic-in-time relaxation, which was recently established for one-dimensional chains. Such relaxation corresponds to the infamous 1/f1/f-noise at strong disorder.Comment: 9 pages, 9 figure

    Oxygen precursor to the reactive intermediate in methanol synthesis by Cu-ZSM-5

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    The reactive oxidizing species in the selective oxidation of methane to methanol in oxygen activated Cu-ZSM-5 was recently defined to be a bent mono(μ-oxo)dicopper(II) species, [Cu_2O]^(2+). In this communication we report the formation of an O_2-precursor of this reactive site with an associated absorption band at 29,000 cm^(-1). Laser excitation into this absorption feature yields a resonance Raman (rR) spectrum characterized by ^(18)O_2 isotope sensitive and insensitive vibrations, νO-O and νCu-Cu, at 736 (Δ^(18)O_2 = 41 cm^(-1)) and 269 cm^(-1), respectively. These define the precursor to be a μ-(η^2:η^2) peroxo dicopper(II) species, [Cu_2(O_2)]^(2+). rR experiments in combination with UV-vis absorption data show that this [Cu_2(O_2)]^(2+) species transforms directly into the [Cu_2O]^(2+) reactive site. Spectator Cu^+ sites in the zeolite ion-exchange sites provide the two electrons required to break the peroxo bond in the precursor. O_2-TPD experiments with ^(18)O_2 show the incorporation of the second ^(18)O atom into the zeolite lattice in the transformation of [Cu_2(O_2)]^(2+) into [Cu_2O]^(2+). This study defines the mechanism of oxo-active site formation in Cu-ZSM-5

    Ligand migration from cluster to support: a crucial factor for catalysis by Thiolate-protected gold clusters

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    Thiolate protected metal clusters are valuable precursors for the design of tailored nanosized catalysts. Their performance can be tuned precisely at atomic level, e.g. by the configuration/ type of ligands or by partial/complete removal of the ligand shell through controlled pre-treatment steps. However, the interaction between the ligand shell and the oxide support, as well as ligand removal by oxidative pre-treatment, are still poorly understood. Typically, it was assumed that the thiolate ligands are simply converted into SO 2 , CO 2 and H 2 O. Herein, we report the first detailed observation of sulfur ligand migration from Au to the oxide support upon deposition and oxidative pre-treatment, employing mainly S K-edge XANES. Conse- quently, thiolate ligand migration not only produces clean Au cluster surfaces but also the surrounding oxide support is modified by sulfur-containing species, with pronounced effects on catalytic propertiesPeer ReviewedPostprint (published version

    Oxygen precursor to the reactive intermediate in methanol synthesis by Cu-ZSM-5

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    The reactive oxidizing species in the selective oxidation of methane to methanol in oxygen activated Cu-ZSM-5 was recently defined to be a bent mono(μ-oxo)dicopper(II) species, [Cu_2O]^(2+). In this communication we report the formation of an O_2-precursor of this reactive site with an associated absorption band at 29,000 cm^(-1). Laser excitation into this absorption feature yields a resonance Raman (rR) spectrum characterized by ^(18)O_2 isotope sensitive and insensitive vibrations, νO-O and νCu-Cu, at 736 (Δ^(18)O_2 = 41 cm^(-1)) and 269 cm^(-1), respectively. These define the precursor to be a μ-(η^2:η^2) peroxo dicopper(II) species, [Cu_2(O_2)]^(2+). rR experiments in combination with UV-vis absorption data show that this [Cu_2(O_2)]^(2+) species transforms directly into the [Cu_2O]^(2+) reactive site. Spectator Cu^+ sites in the zeolite ion-exchange sites provide the two electrons required to break the peroxo bond in the precursor. O_2-TPD experiments with ^(18)O_2 show the incorporation of the second ^(18)O atom into the zeolite lattice in the transformation of [Cu_2(O_2)]^(2+) into [Cu_2O]^(2+). This study defines the mechanism of oxo-active site formation in Cu-ZSM-5

    Ebstein’s anomaly may be caused by mutations in the sarcomere protein gene MYH7

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    Ebstein's anomaly is a rare congenital heart malformation characterised by adherence of the septal and posterior leaflets of the tricuspid valve to the underlying myocardium. Associated abnormalities of left ventricular morphology and function including left ventricular noncompaction (LVNC) have been observed. An association between Ebstein's anomaly with LVNC and mutations in the sarcomeric protein gene MYH7, encoding β-myosin heavy chain, has been shown by recent studies. This might represent a specific subtype of Ebstein's anomaly with a Mendelian inheritance pattern. In this review we discuss the association of MYH7 mutations with Ebstein's anomaly and LVNC and its implications for the clinical care for patients and their family members.Congenital Heart Diseas
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