Determination of 131mXe and 133mXe in the presence of 133gXe via combined beta-spectroscopy and delayed coincidence

The International Monitoring System for the Comprehensive Nuclear-Test-Ban Treaty will include measurements of Xe fission products. Pacific Northwest National Laboratory has developed an automated system for separating Xe from air which detects Xe fission products using a beta-gamma counting system for ^131mXe, ^133mXe, ^133gXe, and ^135gXe. Betas and conversion electrons are detected in a plastic scintillation cell containing the Xe sample. Gamma and X-rays are detected in a NaI(Tl) scintillation detector which surrounds the plastic scintillator sample cell. Two-dimensional pulse-height spectra of gamma-energy versus beta-energy are obtained. The plastic scintillator spectrum in coincidence with the 31-keV X-rays from ^131mXe. ^133mXe, and ^133gXe is a complex mixture of conversion electrons and betas. A new technique to simultaneously measure the delayed coincidence (T _1/2 = 6.27 ns) between beta-particles from ^133gXe and conversion electrons depopulating the 81-keV state in 133 Cs is being developed. This technique allows separation of the ^133gXe beta spectrum from the conversion electrons due to ^131mXe and ^133mXe and uniquely quantifies all three nuclides.     

Adaptive ANOVA decomposition of stochastic incompressible and compressible flows

Realistic representation of stochastic inputs associated with various sources of uncertainty in the simulation of fluid flows leads to high dimensional representations that are computationally prohibitive. We investigate the use of adaptive ANOVA decomposition as an effective dimension–reduction technique in modeling steady incompressible and compressible flows with nominal dimension of random space up to 100. We present three different adaptivity criteria and compare the adaptive ANOVA method against sparse grid, Monte Carlo and quasi-Monte Carlo methods to evaluate its relative efficiency and accuracy. For the incompressible flow problem, the effect of random temperature boundary conditions (modeled as high-dimensional stochastic processes) on the Nusselt number is investigated for different values of correlation length. For the compressible flow, the effects of random geometric perturbations (simulating random roughness) on the scattering of a strong shock wave is investigated both analytically and numerically. A probabilistic collocation method is combined with adaptive ANOVA to obtain both incompressible and compressible flow solutions. We demonstrate that for both cases even draconian truncations of the ANOVA expansion lead to accurate solutions with a speed-up factor of three orders of magnitude compared to Monte Carlo and at least one order of magnitude compared to sparse grids for comparable accuracy.     

Benchmarking the accuracy of coverage-dependent models: adsorption and desorption of benzene on Pt (1 1 1) and Pt3Sn (1 1 1) from first principles

Bimetallic catalysts have demonstrated properties favorable for upgrading biofuel through catalytic hydrodeoxygenation. However, the design and optimization of such bimetallic catalysts requires the ability to construct accurate, predictive models of these systems. To generate a model that predicts the kinetic behavior of benzene adsorbed on Pt (1 1 1) and a Pt₃Sn (1 1 1) surface alloy (Pt₃Sn (1 1 1)), the adsorption of benzene was studied for a wide range of benzene coverages on both surfaces using density functional theory (DFT) calculations. The adsorption energy of benzene was found to correlate linearly with benzene coverage on Pt (1 1 1) and Pt₃Sn (1 1 1); both surfaces exhibited net repulsive lateral interactions. Through an analysis of the d-band properties of the metal surface, it was determined that the coverage dependence is a consequence of the electronic interactions between benzene and the surface. The linear coverage dependence of the adsorption energy allowed us to quantify the influence of the lateral interactions on the heat of adsorption and temperature programmed desorption (TPD) spectra using a mean-field model. A comparison of our simulated TPD to experiment showed that this mean-field model adequately reproduces the desorption behavior of benzene on Pt (1 1 1) and Pt₃Sn (1 1 1). In particular, the TPD correctly exhibits a broadening desorption peak as the initial coverage of benzene increases on Pt (1 1 1) and a low temperature desorption peak on Pt₃Sn (1 1 1). However, due to the sensitivity of the TPD peak temperature to the desorption energy, precise alignment of experimental and theoretical TPD spectra demands an accurate calculation of the adsorption energy. Therefore, an analysis of the effect of the exchange-correlation functional on TPD modeling is presented. Through this work, we show the necessity of incorporating lateral interactions into theoretical models in order to correctly predict experimental behavior.     

Ultrasonic assisted synthesis of palladium-nickel/iron oxide core–shell nanoalloys as effective catalyst for Suzuki-Miyaura and p-nitrophenol reduction reactions

In this study, ultrasonic assisted synthesis of Pd-Ni/Fe₃O₄ core–shell nanoalloys is reported. Unique reaction condition was prepared by ultrasonic irradiation, releasing the stored energy in the collapsed bubbles and heats the bubble contents that leads to Pd(II) and Ni(II) reduction. Co-precipitation method was applied for the synthesis of Fe₃O₄ nanoparticles (NPs). Immobilized solution was produced by sonicating the aqueous mixture of Fe₃O₄ and mercaptosuccinic acid to obtain Pd-Ni alloys on Fe₃O₄ magnetic NP cores. The catalytic activity of the synthesized Pd-Ni/Fe₃O₄ core–shells was investigated in the Suzuki-Miyaura CC coupling reaction and 4-nitrophenol reduction, which exhibited a high catalytic activity in both reactions. These magnetic NPs can be separated from the reaction mixture by external magnetic field. This strategy is simple, economical and promising for industrial applications.     

Acetaldehyde photochemistry on TiO2(1 1 0)

The ultraviolet (UV) photon induced decomposition of acetaldehyde adsorbed on the oxidized rutile TiO₂(1 1 0) surface was studied with photon stimulated desorption (PSD) and thermal programmed desorption (TPD). Acetaldehyde desorbs molecularly from TiO₂(1 1 0) with minor decomposition channels yielding butene on the reduced TiO₂ surface and acetate on the oxidized TiO₂ surface. Acetaldehyde adsorbed on oxidized TiO₂(1 1 0) undergoes a facile thermal reaction to form a photoactive acetaldehyde–oxygen complex. UV irradiation of the acetaldehyde–oxygen complex initiated photofragmentation of the complex resulting in the ejection of methyl radical into gas phase and conversion of the surface bound fragment to formate.     

High resolution analysis of the rotational levels of the (0 0 0), (0 1 0), (1 0 0), (0 0 1), (0 2 0), (1 1 0) and (0 1 1) vibrational states of SO2

A high resolution (0.0018 cm⁻¹) Fourier transform instrument has been used to record the spectrum of an enriched ³⁴S (95.3%) sample of sulfur dioxide. A thorough analysis of the ν₂, 2ν₂ − ν₂, ν₁, ν₁ + ν₂ − ν₂, ν₃, ν₂ + ν₃ − ν₂, ν₁ + ν₂ and ν₂ + ν₃ bands has been carried out leading to a large set of assigned lines. From these lines ground state combination differences were obtained and fit together with the existing microwave, millimeter, and terahertz rotational lines. An improved set of ground state rotational constants were obtained. Next, the upper state rotational levels were fit. For the (0 1 0), (1 1 0) and (0 1 1) states, a simple Watson-type Hamiltonian sufficed. However, it was necessary to include explicitly interacting terms in the Hamiltonian matrix in order to fit the rotational levels of the (0 2 0), (1 0 0) and (1 0 1) states to within their experimental accuracy. More explicitly, it was necessary to use a ΔK = 2 term to model the Fermi interaction between the (0 2 0) and (1 0 0) levels and a ΔK = 3 term to model the Coriolis interaction between the (1 0 0) and (0 0 1) levels. Precise Hamiltonian constants were derived for the (0 0 0), (0 1 0), (1 0 0), (0 0 1), (0 2 0), (1 1 0) and (0 1 1) vibrational states.     

磁瓶式光电子能谱和速度成像光电子能谱对APS-(A=C14H10,蒽)的研究:电子结构,APS·的自旋轨道耦合和APS-的自旋偶极态

Gaseous dibenzo-7-phosphanorbornadiene P-sulfide anions APS^-(A=C₁₄H₁₀ or anthracene) were generated via electrospray ionization, and characterized by magnetic-bottle photoelectron spectroscopy, velocity-map imaging (VMI) photoelectron spectroscopy, and quantum chemical calculations. The electron affinity (EA) and spin-orbit (SO) splitting of the APS^· radical are determined from the photoelectron spectra and Franck-Condon factor simulations to be EA=(2.62±0.05) eV and SO splitting=(43±7) meV. VMI photoelectron images show strong and sharp peaks near the detachment threshold with an identical electron kinetic energy (eKE) of 17.9 meV at three different detachment wavelengths, which are therefore assigned to autodetachment from dipole-bound anion states. The B3LYP/6-31++G(d,p) calculations indicate APS^· has a dipole moment of 3.31 Debye, large enough to support a dipole-bound electron.     

The Quantum Cellular Automaton as a Markov Process

The dynamical behavior of the Quantum Cellular Automaton (QCA) is described here as a Markov Process. Ergodicity and recurrence, emergent properties of the discrete dynamical QCA system, are defined in the context of the characteristic polynomial of the Markov transition matrix. Except for a few anomalous cases, the transition matrix can be used to predict recurrence times. Finally, a correspondence between recurrence and elementary particle mass is proposed as an example of an emergent property of the QCA system. © 1999 Elsevier Science Ltd. All rights reserved.     

Behavior of CO2/water flow in porous media for CO2 geological storage

A clear understanding of two-phase fluid flow properties in porous media is of importance to CO₂ geological storage. The study visually measured the immiscible and miscible displacement of water by CO₂ using MRI (magnetic resonance imaging), and investigated the factor influencing the displacement process in porous media which were filled with quartz glass beads. For immiscible displacement at slow flow rates, the MR signal intensity of images increased because of CO₂ dissolution; before the dissolution phenomenon became inconspicuous at flow rate of 0.8 mL min^− 1. For miscible displacement, the MR signal intensity decreased gradually independent of flow rates, because supercritical CO₂ and water became miscible in the beginning of CO₂ injection. CO₂ channeling or fingering phenomena were more obviously observed with lower permeable porous media. Capillary force decreases with increasing particle size, which would increase permeability and allow CO₂ and water to invade into small pore spaces more easily. The study also showed CO₂ flow patterns were dominated by dimensionless capillary number, changing from capillary finger to stable flow. The relative permeability curve was calculated using Brooks-Corey model, while the results showed the relative permeability of CO₂ slightly decreases with the increase of capillary number.