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451.
Lee Y He G Akey AJ Si R Flytzani-Stephanopoulos M Herman IP 《Journal of the American Chemical Society》2011,133(33):12952-12955
Oxygen vacancy levels are monitored during the oxidation of CO by CeO(2-δ) nanorods and Au-CeO(2-δ) nanorods, nanocubes, and nanopolyhedra by using Raman scattering. The first-order CeO(2) F(2g) peak near 460 cm(-1) decreases when this reaction is fast (fast reduction and relatively slow reoxidation of the surface), because of the lattice expansion that occurs when Ce(3+) replaces Ce(4+) during oxygen vacancy creation. This shift correlates with reactivity for CO oxidation. Increases in the oxygen deficit δ as large as ~0.04 are measured relative to conditions when the ceria is not reduced. 相似文献
452.
Cyphersmith A Surampudi S Casey MJ Jankowski K Venkataraman D Barnes MD 《The journal of physical chemistry. A》2012,116(22):5349-5352
We report on the single-molecule chiroptical properties of "right"-handed bridged triaryl amine helicene dimers, MH2. Using an experimental setup to precisely define the circular excitation polarization at the sample plane, we investigated the circular dichroic response in luminescence from individual molecules in which induced ellipticity from microscope optics is minimized. Our results comparing circular anisotropies in fluorescence excitation from MH2 and perylene diimide (PDI), an achiral, centrosymmetric chromophore, demonstrate a significant reduction in the breadth of the distribution of circular dissymmetry parameters obtained from modulation of the circularly polarized excitation source (457 nm). For PDI, we observe a symmetric distribution of circular anisotropy parameters centered about zero, with a fwhm of 0.25. For MH2, we observe an asymmetric distribution peaked at g = -0.09, with a slightly larger width as the corresponding PDI distribution. These results indicate that the large dissymmetry parameters (|g| > 0.5) in fluorescence excitation described in our original report (Hassey, R.; et al. Chirality 2008, 20, 1039-1046 and Hassey, R.; et al. Science 2006, 314, 1437-1439) were indeed affected by (at the time, unknown) linear polarization artifacts. However, the present results on MH2 provide compelling evidence for single-molecule circular dissymmetries much larger than solution or thin-film ensemble values, defined primarily by the enhanced rotatory strength (relative to the monomer), and restricted orientation at the sample surface. 相似文献
453.
454.
We have performed detailed SIMION simulations of ion behavior in micrometer-sized cylindrical ion traps (r0 = 1 microm). Simulations examined the effects of ion and neutral temperature, the pressure and nature of cooling gas, ion mass, trap voltage and frequency, space-charge, fabrication defects, and other parameters on the ability of micrometer-sized traps to store ions. At this size scale voltage and power limitations constrain trap operation to frequencies about 1 GHz and rf amplitudes of tens of volts. Correspondingly, the pseudopotential well depth of traps is shallow, and thermal energies contribute significantly to ion losses. Trapping efficiency falls off gradually as qz approaches 0.908, possibly complicating mass-selective trapping, ejection, or quantitation. Coulombic repulsion caused by multiple ions in a small-volume results in a trapping limit of a single ion per trap. If multiple ions are produced in a trap, all but one ion are ejected within a few microseconds. The remaining ion tends to have favorable trapping parameters and a lifetime about hundreds of microseconds; however, this lifetime is significantly shorter than it would have been in the absence of space-charge. Typical microfabrication defects affect ion trapping only minimally. We recently reported (IJMS 2004, 236, 91-104) on the construction of a massively parallel array of ion traps with dimensions of r0 = 1 microm. The relationship of the simulations to the expected performance of the microfabricated array is discussed. 相似文献
455.
456.
Determination of complex mixtures of volatile organic compounds in ambient air: canister methodology
Canister methodology is applicable to 150 polar and nonpolar VOCs found in ambient air from parts-per-billion by volume (ppbv)
to parts-per-million (ppmv) levels, and has been validated at parts-per-trillion (pptv) levels for a subset of these analytes.
This article is a detailed review of techniques related to the collection of volatile organic compounds (VOCs) in evacuated
Summa and fused-silica-lined canisters, and their analysis by gas chromatography/mass spectrometry (GC/MS). Emphasis is placed
on canister cleaning, VOC stability in canisters, sample dilution, water management, and VOC cryogenic and sorbent preconcentration
methods. A wide range of VOC preconcentration and water management methods are identified from the literature, and their relative
merits and disadvantages are discussed. Examples of difficulties that commonly arise when processing canister samples are
illustrated, and solutions to these problems are provided. 相似文献
457.
"Rung 3.5" exchange-correlation functionals for Kohn-Sham density functional theory depend linearly on the nonlocal one-particle density matrix of the noninteracting Kohn-Sham reference system. Rung 3.5 functionals also require a semilocal model for the one-particle density matrix. This work presents new model density matrices for Rung 3.5 functionals. The resulting functionals give reasonable predictions for total energies, molecular thermochemistry and kinetics, odd-electron bonds, and conjugated polymer bandgaps. Global-hybrid-like combinations of semilocal and Rung 3.5 exchange, and empirical density matrix models, also show promise. 相似文献
458.
Matthew D. Blair G. Austin Ford Sebastian Herr Jeremy L. Marzuola 《Journal of Geometric Analysis》2012,22(2):339-351
We prove Strichartz estimates with a loss of derivatives for the Schrödinger equation on polygonal domains with either Dirichlet or Neumann homogeneous boundary conditions. Using a standard doubling procedure, estimates on the polygon follow from those on Euclidean surfaces with conical singularities. We develop a Littlewood-Paley squarefunction estimate with respect to the spectrum of the Laplacian on these spaces. This allows us to reduce matters to proving estimates at each frequency scale. The problem can be localized in space provided the time intervals are sufficiently small. Strichartz estimates then follow from a recent result of the second author regarding the Schrödinger equation on the Euclidean cone. 相似文献
459.
Robert E. Majewski Alan S. Edelstein Austin E. Dwight 《Solid State Communications》1979,31(5):315-320
Susceptibility measurements taken for 1.5 ≤ T ≤ 17 K on the system CexLa1?xAl3 indicate that the Ce moment is nearly stabilized on dilution. Evidence for this is the fact that the fractional occupancy of the 4f1 configuration and the spin correlation time both increase as x → 0. Crystalline electric fields influence the susceptibility of these valence fluctuation systems. 相似文献
460.
John T. Gupton Robert B. Miller Stuart C. Clough Rene P.F. Kanters Kartik M. Keertikar John M. Solano Daniel W. Callahan Austin B. Scharf 《Tetrahedron》2005,61(7):1845-1854
A new and efficient relay synthesis of the marine natural products polycitone A and B is described. The new strategy relies on the formation of 2,4-disubstituted pyrroles from a vinamidinium salt followed by electrophilic substitution at the 5-position of the pyrrole and Suzuki coupling at the 4-position to produce the tetrasubstituted heterocycle efficiently and with complete control of regiochemistry. 相似文献