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Synthesis and Study of Olefin Metathesis Catalysts Supported by Redox-Switchable Diaminocarbene 3 Ferrocenophanes
A redox-switchable ligand, N,N'-dimethyldiaminocarbene[3]ferrocenophane (5), was synthesized and incorporated into a series of Ir- and Ru-based complexes. Electrochemical and spectroscopic analyses of (5) Ir(CO)(2)Cl (15) revealed that 5 displayed a Tolman electronic parameter value of 2050 cm(-1) in the neutral state and 2061 cm(-1) upon oxidation. Moreover, inspection of X-ray crystallography data recorded for (5) Ir(cis,cis-1,5-cyclooctadiene)Cl (13) revealed that 5 was sterically less bulky (%V-Bur = 28.4) than other known diaminocarbene[3]ferrocenophanes, which facilitated the synthesis of (5)(PPh3)Cl2Ru-(3-phenylindenylid-1-ene) (18). Complex 18 exhibited quasi-reversible electrochemical processes at 0.79 and 0.98 V relative to SCE, which were assigned to the Fe and Ru centers in the complex, respectively, based on UV-vis and electron pair resonance spectroscopic measurements. Adding 2,3-dichloro-5,6-dicyanoquinone over the course of a ring-opening metathesis polymerization of cis, cis-1,5-cyclooctadiene catalyzed by 18 ([monomer](0)/[18](0) = 2500) reduced the corresponding rate constant of the reaction by over an order of magnitude (pre-oxidation: k(obs) = 0.045 s(-1); post-oxidation: k(obs) = 0.0012 s(-1)). Subsequent reduction of the oxidized species using decamethylferrocene restored catalytic activity (post-reduction: k(obs) = up to 0.016 s(-1), depending on when the reductant was added). The difference in the polymerization rates was attributed to the relative donating ability of the redox-active ligand (i.e., strongly donating 5 versus weakly donating 5(+)) which ultimately governed the activity displayed by the corresponding catalyst.U. S. Army Research Office W911NF-09-1-0446Chemistr
ORFEUS II and IUE Spectroscopy of EX Hydrae
Using ORFEUS-SPAS II FUV spectra, IUE UV spectra, and archival EUVE deep
survey photometry, we present a detailed picture of the behavior of the
magnetic cataclysmic variable EX Hydrae. Like HUT spectra of this source, the
FUV and UV spectra reveal broad emission lines of He II, C II-IV, N III and V,
O VI, Si III-IV, and Al III superposed on a continuum which is blue in the UV
and nearly flat in the FUV. Like ORFEUS spectra of AM Her, the O VI doublet is
resolved into broad and narrow emission components. Consistent with its
behavior in the optical, the FUV and UV continuum flux densities, the FUV and
UV broad emission line fluxes, and the radial velocity of the O VI broad
emission component all vary on the spin phase of the white dwarf, with the
maximum of the FUV and UV continuum and broad emission line flux light curves
coincident with maximum blueshift of the broad O VI emission component. On the
binary phase, the broad dip in the EUV light curve is accompanied by strong
eclipses of the UV emission lines and by variations in both the flux and radial
velocity of the O VI narrow emission component. The available data are
consistent with the accretion funnel being the source of the FUV and UV
continuum and the O VI broad emission component, and the white dwarf being the
source of the O VI narrow emission component.Comment: 21 pages, 10 Postscript figures; LaTeX format, uses aaspp4.sty;
table2.tex included separately because it must be printed sideways - see
instructions in the file; accepted on 1999 Feb 20 for publication in The
Astrophysical Journa
A Quantitative Non-radial Oscillation Model for the Subpulses in PSR B0943+10
In this paper, we analyze time series measurements of PSR B0943+10 and fit
them with a non-radial oscillation model. The model we apply was first
developed for total intensity measurements in an earlier paper, and expanded to
encompass linear polarization in a companion paper to this one. We use PSR
B0943+10 for the initial tests of our model because it has a simple geometry,
it has been exhaustively studied in the literature, and its behavior is
well-documented. As prelude to quantitative fitting, we have reanalyzed
previously published archival data of PSR B0943+10 and uncovered subtle but
significant behavior that is difficult to explain in the framework of the
drifting spark model. Our fits of a non-radial oscillation model are able to
successfully reproduce the observed behavior in this pulsar.Comment: 45 pages, 16 figures, accepted Ap
Uncivil behaviour in the workplace causes mental fatigue and is contagious
Employees on the receiving end tend to ‘pay forward’ the incivility to others, write Christopher C. Rosen, Joel Koopman, Allison S. Gabriel and Russell E. Johnso
A new family of S-folds in type IIB string theory
We construct infinite new classes of solutions of
type IIB string theory which have non-trivial monodromy
along the direction. The solutions are supersymmetric and holographically
dual, generically, to SCFTs in . The solutions are first
constructed as solutions in gauged
supergravity and then uplifted to . The solutions all arise as limiting
cases of Janus solutions of , SYM theory which are
supported both by a different value of the coupling constant on either side of
the interface, as well as by fermion and boson mass deformations. As special
cases, the construction recovers three known S-fold constructions, which
preserve and 4 supersymmetry, as well as a recently
constructed solution (not
S-folded). We also present some novel "one-sided Janus" solutions that are
non-singular.Comment: 54 pages, 13 figure
Liat1, an arginyltransferase-binding protein whose evolution among primates involved changes in the numbers of its 10-residue repeats
The arginyltransferase Ate1 is a component of the N-end rule pathway, which recognizes proteins containing N-terminal degradation signals called N-degrons, polyubiquitylates these proteins, and thereby causes their degradation by the proteasome. At least six isoforms of mouse Ate1 are produced through alternative splicing of Ate1 pre-mRNA. We identified a previously uncharacterized mouse protein, termed Liat1 (ligand of Ate1), that interacts with Ate1 but does not appear to be its arginylation substrate. Liat1 has a higher affinity for the isoforms Ate1^(1A7A) and Ate1^(1B7A). Liat1 stimulated the in vitro N-terminal arginylation of a model substrate by Ate1. All examined vertebrate and some invertebrate genomes encode proteins sequelogous (similar in sequence) to mouse Liat1. Sequelogs of Liat1 share a highly conserved ∼30-residue region that is shown here to be required for the binding of Liat1 to Ate1. We also identified non-Ate1 proteins that interact with Liat1. In contrast to Liat1 genes of nonprimate mammals, Liat1 genes of primates are subtelomeric, a location that tends to confer evolutionary instability on a gene. Remarkably, Liat1 proteins of some primates, from macaques to humans, contain tandem repeats of a 10-residue sequence, whereas Liat1 proteins of other mammals contain a single copy of this motif. Quantities of these repeats are, in general, different in Liat1 of different primates. For example, there are 1, 4, 13, 13, 17, and 17 repeats in the gibbon, gorilla, orangutan, bonobo, neanderthal, and human Liat1, respectively, suggesting that repeat number changes in this previously uncharacterized protein may contribute to evolution of primates
An Improved Methodology for Multidimensional High- Throughput Preformulation Characterization of Protein Conformational Stability
The Empirical Phase Diagram (EPD) technique is a vector-based multidimensional analysis method for summarizing large data sets from a variety of biophysical techniques. It can be used to provide comprehensive preformulation characterization of a macromolecule’s higher-order structural integrity and conformational stability. In its most common mode, it represents a type of stimulus-response diagram using environmental variables such as temperature, pH, and ionic strength as the stimulus, with alterations in macromolecular structure being the response. Until now EPD analysis has not been available in a high throughput mode because of the large number of experimental techniques and environmental stressor/stabilizer variables typically employed. A new instrument has been developed that combines circular dichroism, UV-absorbance, fluorescence spectroscopy and light scattering in a single unit with a 6-position temperature controlled cuvette turret. Using this multifunctional instrument and a new software system we have generated EPDs for four model proteins. Results confirm the reproducibility of the apparent phase boundaries and protein behavior within the boundaries. This new approach permits two EPDs to be generated per day using only 0.5 mg of protein per EPD. Thus, the new methodology generates reproducible EPDs in high-throughput mode, and represents the next step in making such determinations more routine
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