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Chronology of CH···O Hydrogen Bonding from Molecular Dynamics Studies of the Phosphoric Acid-Catalyzed Allylboration of Benzaldehyde
CH···O hydrogen bonds involving formyl groups have been invoked as a crucial factor controlling many asymmetric transformations. We conducted quasi-classical direct molecular dynamics simulations on the phosphoric acid-catalyzed allylboration of benzaldehyde to understand the synergy between the phosphoric acid OH···O hydrogen bond and the secondary CH···O formyl hydrogen bond as the reaction occurs. In the gas phase, both the CH···O and OH···O hydrogen bonds are enhanced from reactants to transition states. In toluene, the trend of H-bond enhancement is observed with a smaller magnitude because of solvent caging. The strength of the formyl hydrogen bond in the TS, a second CH···O interaction between the P═O oxygen and -hydrogen of the phenyl ring and the OH···O hydrogen bond were determined using quantum mechanical calculations (4.6, 1.0, and 14.5 kcal mol, respectively).We are grateful to The English-Speaking Union (Lindemann Trust Fellowship to M.N.G.), Girton College, Cambridge (Research Fellowship to M.N.G.) and the NSF (CHE-1361104 to K.N.H.) for financial support. Computational resources were provided by the UCLA Institute for Digital Research and Education (IDRE) and the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by the NSF (OCI-1053575)
Electrostatics of Edge States of Quantum Hall Systems with Constrictions: Metal--Insulator Transition Tuned by External Gates
The nature of a metal--insulator transition tuned by external gates in
quantum Hall (QH) systems with point constrictions at integer bulk filling, as
reported in recent experiments of Roddaro et al. [1], is addressed. We are
particularly concerned here with the insulating behavior--the phenomena of
backscattering enhancement induced at high gate voltages. Electrostatics
calculations for QH systems with split gates performed here show that
observations are not a consequence of interedge interactions near the point
contact. We attribute the phenomena of backscattering enhancement to a
splitting of the integer edge into conducting and insulating stripes, which
enable the occurrence of the more relevant backscattering processes of
fractionally charged quasiparticles at the point contact. For the values of the
parameters used in the experiments we find that the conducting channels are
widely separated by the insulating stripes and that their presence alters
significantly the low-energy dynamics of the edges. Interchannel impurity
scattering does not influence strongly the tunneling exponents as they are
found to be irrelevant processes at low energies. Exponents of backscattering
at the point contact are unaffected by interchannel Coulomb interactions since
all channels have same chirality of propagation.Comment: 19 pages; To appear in Phys. Rev.
Comparison of AlloDerm and AlloMax tissue incorporation in rats.
BackgroundHuman acellular dermal matrices (HADMs) are used in a variety of settings. AlloMax is a new HADM currently being used for breast reconstruction and hernia repair. We compared the in vivo tissue integration of AlloMax to AlloDerm, a well-studied HADM, in rats.MethodsWe implanted AlloDerm and AlloMax patches into subcutaneous pockets on the backs of 32 male Sprague-Dawley rats. The animals were killed after either 4 or 8 weeks, and the patches were recovered and stained for histopathologic analyses. Microscopic end points included patch thickness, vascularization, tissue in-growth, fibroblast proliferation, and inflammation.ResultsAll animals completed the study without complications or infection. There were no significant differences in graft thicknesses at 4 and 8 weeks. Microscopically, at 4 weeks, AlloDerm sections had significantly more microvessels than AlloMax (P = 0.02). This disparity increased by 8 weeks (P < 0.01). Similarly, we found greater tissue in-growth and fibroblast proliferation in AlloDerm than AlloMax sections at 4 (P < 0.01) and at 8 (P < 0.01) weeks. Inflammatory infiltrates consisted of lymphocytes, histiocytes, eosinophils, and plasma cells. Deep graft infiltration by predominately lymphocytic inflammatory cells was significantly higher in AlloDerm than AlloMax grafts at 4 (P = 0.01) and 8 (P = 0.02) weeks. Graft necrosis was uncommon, but marginal fibrosis was similar in both.ConclusionsAlloDerm grafts had greater neovascularization, tissue infiltration, fibroblast proliferation, and inflammatory reaction than AlloMax grafts when placed subcutaneously in rats. AlloDerm may be better incorporated than AlloMax when placed in vivo
Evolution of Landau Levels into Edge States at an Atomically Sharp Edge in Graphene
The quantum-Hall-effect (QHE) occurs in topologically-ordered states of
two-dimensional (2d) electron-systems in which an insulating bulk-state
coexists with protected 1d conducting edge-states. Owing to a unique
topologically imposed edge-bulk correspondence these edge-states are endowed
with universal properties such as fractionally-charged quasiparticles and
interference-patterns, which make them indispensable components for QH-based
quantum-computation and other applications. The precise edge-bulk
correspondence, conjectured theoretically in the limit of sharp edges, is
difficult to realize in conventional semiconductor-based electron systems where
soft boundaries lead to edge-state reconstruction. Using scanning-tunneling
microscopy and spectroscopy to follow the spatial evolution of bulk
Landau-levels towards a zigzag edge of graphene supported above a graphite
substrate we demonstrate that in this system it is possible to realize
atomically sharp edges with no edge-state reconstruction. Our results single
out graphene as a system where the edge-state structure can be controlled and
the universal properties directly probed.Comment: 16 pages, 4 figure
Hall effect in the marginal Fermi liquid regime of high-Tc superconductors
The detailed derivation of a theory for transport in quasi-two-dimensional
metals, with small-angle elastic scattering and angle-independent inelastic
scattering is presented. The transport equation is solved for a model Fermi
surface representing a typical cuprate superconductor. Using the small-angle
elastic and the inelastic scattering rates deduced from angle-resolved
photoemission experiments, good quantitative agreement with the observed
anomalous temperature dependence of the Hall angle in optimally doped cuprates
is obtained, while the resistivity remains linear in temperature. The theory is
also extended to the frequency-dependent complex Hall angle
Infrared Hall effect in high Tc superconductors: Evidence for non-Fermi liquid Hall scattering
Infrared (20-120 cm-1 and 900-1100 cm-1) Faraday rotation and circular
dichroism are measured in high Tc superconductors using sensitive polarization
modulation techniques. Optimally doped YBCO thin films are studied at
temperatures down to 15 K and magnetic fields up to 8 T. At 1000 cm-1 the Hall
conductivity varies strongly with temperature in contrast to the longitudinal
conductivity which is nearly independent of temperature. The Hall scattering
rate has a T^2 temperature dependence but, unlike a Fermi liquid, depends only
weakly on frequency. The experiment puts severe constraints on theories of
transport in the normal state of high Tc superconductors.Comment: 8 pages, 3 figure
BICEP3 performance overview and planned Keck Array upgrade
Bicep3 is a 520mm aperture, compact two-lens refractor designed to observe the polarization of the cosmic microwave background (CMB) at 95 GHz. Its focal plane consists of modularized tiles of antenna-coupled transition edge sensors (TESs), similar to those used in Bicep2 and the Keck Array. The increased per-receiver optical throughput compared to Bicep2/Keck Array, due to both its faster f=1:7 optics and the larger aperture, more than doubles the combined mapping speed of the Bicep/Keck program. The Bicep3 receiver was recently upgraded to a full complement of 20 tiles of detectors (2560 TESs) and is now beginning its second year of observation (and first science season) at the South Pole. We report on its current performance and observing plans. Given its high per-receiver throughput while maintaining the advantages of a compact design, Bicep3- class receivers are ideally suited as building blocks for a 3rd-generation CMB experiment, consisting of multiple receivers spanning 35 GHz to 270 GHz with total detector count in the tens of thousands. We present plans for such an array, the new "BICEP Array" that will replace the Keck Array at the South Pole, including design optimization, frequency coverage, and deployment/observing strategies
High-density information storage in an absolutely defined aperiodic sequence of monodisperse copolyester
Synthesis of a polymer composed of a large discrete number of chemically distinct monomers in an absolutely defined aperiodic sequence remains a challenge in polymer chemistry. The synthesis has largely been limited to oligomers having a limited number of repeating units due to the difficulties associated with the step-by-step addition of individual monomers to achieve high molecular weights. Here we report the copolymers of ??-hydroxy acids, poly(phenyllactic-co-lactic acid) (PcL) built via the cross-convergent method from four dyads of monomers as constituent units. Our proposed method allows scalable synthesis of sequence-defined PcL in a minimal number of coupling steps from reagents in stoichiometric amounts. Digital information can be stored in an aperiodic sequence of PcL, which can be fully retrieved as binary code by mass spectrometry sequencing. The information storage density (bit/Da) of PcL is 50% higher than DNA, and the storage capacity of PcL can also be increased by adjusting the molecular weight (~38???kDa)
BICEP3: a 95 GHz refracting telescope for degree-scale CMB polarization
BICEP3 is a 550 mm-aperture refracting telescope for polarimetry of radiation
in the cosmic microwave background at 95 GHz. It adopts the methodology of
BICEP1, BICEP2 and the Keck Array experiments - it possesses sufficient
resolution to search for signatures of the inflation-induced cosmic
gravitational-wave background while utilizing a compact design for ease of
construction and to facilitate the characterization and mitigation of
systematics. However, BICEP3 represents a significant breakthrough in
per-receiver sensitivity, with a focal plane area 5 larger than a
BICEP2/Keck Array receiver and faster optics ( vs. ).
Large-aperture infrared-reflective metal-mesh filters and infrared-absorptive
cold alumina filters and lenses were developed and implemented for its optics.
The camera consists of 1280 dual-polarization pixels; each is a pair of
orthogonal antenna arrays coupled to transition-edge sensor bolometers and read
out by multiplexed SQUIDs. Upon deployment at the South Pole during the 2014-15
season, BICEP3 will have survey speed comparable to Keck Array 150 GHz (2013),
and will significantly enhance spectral separation of primordial B-mode power
from that of possible galactic dust contamination in the BICEP2 observation
patch.Comment: 12 pages, 5 figures. Presented at SPIE Astronomical Telescopes and
Instrumentation 2014: Millimeter, Submillimeter, and Far-Infrared Detectors
and Instrumentation for Astronomy VII. To be published in Proceedings of SPIE
Volume 915
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