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Heaven M.C.,Emory University | Barker B.J.,Los Alamos National Laboratory | Antonov I.O.,Combustion Research Facility
Journal of Physical Chemistry A | Year: 2014

Understanding the influence of electrons in partially filled f- and d-orbitals on bonding and reactivity is a key issue for actinide chemistry. This question can be investigated by using a combination of well-defined experimental measurements and theoretical calculations. Gas phase spectroscopic data are particularly valuable for the evaluation of theoretical models. Consequently, the primary objectives of our research have been to obtain gas phase spectra for small actinide molecules. To complement the experimental effort, we are investigating the potential for using relativistic ab initio calculations and semiempirical models to predict and interpret the electronic energy level patterns for f-element compounds. Multiple resonance spectroscopy and jet cooling techniques have been used to unravel the complex electronic spectra of Th and U compounds. Recent results for fluorides, sulfides, and nitrides are discussed. (Figure Presented). © 2014 American Chemical Society. Source

O'Connor J.,Combustion Research Facility | Lieuwen T.,Georgia Institute of Technology
Physics of Fluids | Year: 2012

This work investigates the response of the vortex breakdown region of a swirling, annular jet to transverse acoustic excitation for both non-reacting and reacting flows. This swirling flow field consists of a central vortex breakdown region, two shear layers, and an annular fluid jet. The vortex breakdown bubble, a region of highly turbulent recirculating flow in the center of the flowfield, is the result of a global instability of the swirling jet. Additionally, the two shear layers originating from the inner and outer edge of the annular nozzle are convectively unstable and rollup due to the Kelvin-Helmholtz instability. Unlike the convectively unstable shear layers that respond in a monotonic manner to acoustic forcing, the recirculation zone exhibits a range of response characteristics, ranging from minimal response to exhibiting abrupt bifurcations at large forcing amplitudes. In this study, the response of the time-average and fluctuating recirculation zone is measured as a function of forcing frequency, amplitude, and symmetry. The time-average flow field is shown to exhibit both monotonically varying and abrupt bifurcation features as acoustic forcing amplitude is increased. The unsteady motion in the recirculation zone is dominated by the low frequency precession of the vortex breakdown bubble. In the unforced flow, the azimuthal m = -2 and m = -1 modes (i.e., disturbances rotating in the same direction as the swirl flow) dominate the velocity disturbance field. These modes correspond to large scale deformation of the jet column and two small-scale precessing vortical structures in the recirculation zone, respectively. The presence of high amplitude acoustic forcing changes the relative amplitude of these two modes, as well as the character of the self-excited motion. For the reacting flow problem, we argue that the direct effect of these recirculation zone fluctuations on the flame response to flow forcing is not significant. Rather, flame wrinkling in response to flow forcing is dominated by shear layer disturbances. Recirculation zone dynamics primarily influence the time-average flame features (such as spreading angle). These influences on the flame response are indirect, as they control the transfer function relating shear layer fluctuations and the resulting flame response. © 2012 American Institute of Physics. Source

A counterpropagating phase-matching geometry is employed for high-spatial-resolution one-dimensional (1D) imaging of temperature and O 2-to-N2 concentration ratio using picosecond pure-rotational coherent anti-Stokes Raman spectroscopy (RCARS) over a large field (20 mm). A single-shot 1D RCARS image of more than 20 mm in length is thus acquired at 300 K in air. High-resolution 1D RCARS flame measurements are demonstrated using a custombuilt burner and a premixed methane/air flame (Φ = 0.6). This phase-matching scheme improves the spatial resolution by approximately 1 order of magnitude when compared to the standard small-angle BOXCARS phase-matching schemes typically employed in CARS measurements. Additionally, for a 20 mm 1D image, signal levels are increased by 10 2 because of the higher irradiance provided in the current scheme. © 2012 Optical Society of America. Source

Knudsen E.,Stanford University | Richardson E.S.,University of Southampton | Doran E.M.,Robert Bosch GmbH | Pitsch H.,Institute For Technische Verbrennung | Chen J.H.,Combustion Research Facility
Physics of Fluids | Year: 2012

Scalar dissipation rates and subfilter scalar variances are important modeling parameters in large eddy simulations (LES) of reacting flows. Currently available models capture the general behavior of these parameters, but these models do not always perform with the degree of accuracy that is needed for predictive LES. Here, two direct numerical simulations (DNS) are used to analyze LES dissipation rate and variance modelsto propose a new model for the dissipation rate that is based on a transport equation. The first DNS that is considered is a non-premixed auto-igniting C2H4 jet flame simulation originally performed by Yoo et al. [Proc. Combust. Inst.33, 1619-1627 (2011)]10.1016/j.proci.2010.06.147. A LES of this case is run using algebraic models for the dissipation rate and subfilter variance. It is shown that the algebraic models fail to adequately reproduce the DNS results. This motivates the introduction of a transport equation model for the LES dissipation rate. Closure of the equation is addressed by formulating a new adapted dynamic approach. This approach borrows dynamically computed information from LES quantities that, unlike the dissipation rate, do not reside on the smallest flow length scales. The adapted dynamic approach is analyzed by considering a second DNS of scalar mixing in homogeneous isotropic turbulence. Data from this second DNS are used to confirm that the adapted dynamic approach successfully closes the dissipation rate equation over a wide range of LES filter widths. The first reacting jet case is then returned to and used to test the LES transport equation models. The transport equation model for the dissipation rate is shown to be more accurate than its algebraic counterpointthe dissipation rate is eliminated as a source of error in the transported variance model. © 2012 American Institute of Physics. Source

Magnotti G.,Combustion Research Facility | Cutler A.D.,George Washington University | Danehy P.M.,NASA
Applied Optics | Year: 2013

This work describes the development of a dual-pump coherent anti-Stokes Raman spectroscopy system for simultaneous measurements of the temperature and the absolute mole fraction of N2, O2, and H2 in supersonic combusting flows. Changes to the experimental setup and the data analysis to improve the quality of the measurements in this turbulent, high-temperature reacting flow are described. The accuracy and precision of the instrument have been determined using data collected in a Hencken burner flame. For temperatures above 800 K, errors in the absolute mole fraction are within 1.5%, 0.5%, and 1% of the total composition for N2, O2, and H2, respectively. Standard deviations based on 500 single shots are between 10 and 65 K for the temperature, between 0.5% and 1.7% of the total composition for O2, and between 1.5% and 3.4% for N2. The standard deviation of H2 is ∼10% of the average measured mole fraction. © 2013 Optical Society of America. Source

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