We report pulsed dielectric barrier discharges (DBD) in He–H2O and He–H2O–O2 mixtures are studied in near atmospheric conditions using temporally and spatially resolved quantitative 2D imaging of the hydroxyl radical (OH) and hydrogen peroxide (H2O2 ). The primary goal was to detect and quantify the production of these strongly oxidative species in water-laden helium discharges in a DBD jet configuration, which is of interest for biomedical applications such as disinfection of surfaces and treatment of biological samples. Hydroxyl profiles are obtained by laser-induced fluorescence (LIF) measurements using 282 nm laser excitation. Hydrogen peroxide profiles are measured by photo-fragmentation LIF (PF-LIF), which involves photo-dissociating H2O2 into OH with a 212.8 nm laser sheet and detecting the OH fragments by LIF. The H2O2 profiles are calibrated by measuring PF-LIF profiles in a reference mixture of He seeded with a known amount of H2O2 . OH profiles are calibrated by measuring OH-radical decay times and comparing these with predictions from a chemical kinetics model. Two different burst discharge modes with five and ten pulses per burst are studied, both with a burst repetition rate of 50 Hz. In both cases, dynamics of OH and H2O2 distributions in the afterglow of the discharge are investigated. Gas temperatures determined from the OH-LIF spectra indicate that gas heating due to the plasma is insignificant. The addition of 5% O2 in the He admixture decreases the OH densities and increases the H2O2 densities. The increased coupled energy in the ten-pulse discharge increases OH and H2O2 mole fractions, except for the H2O2 in the He–H2O–O2 mixture which is relatively insensitive to the additional pulses.
The methyl radical plays a central role in plasma-assisted hydrocarbon chemistry but is challenging to detect due to its high reactivity and strongly pre-dissociative electronically excited states. In this work, we report the development of a photo-fragmentation laser-induced fluorescence (PF-LIF) diagnostic for quantitative 2D imaging of methyl profiles in a plasma. This technique provides temporally and spatially resolved measurements of local methyl distributions, including in near-surface regions that are important for plasma-surface interactions such as plasma-assisted catalysis. The technique relies on photo-dissociation of methyl by the fifth harmonic of a Nd:YAG laser at 212.8 nm to produce CH fragments. These photofragments are then detected with LIF imaging by exciting a transition in the B-X(0, 0) band of CH with a second laser at 390 nm. Fluorescence from the overlapping A-X(0, 0), A-X(1, 1), and B-X(0, 1) bands of CH is detected near 430 nm with the A-state populated by collisional B-A electronic energy transfer. This non-resonant detection scheme enables interrogation close to a surface. The PF-LIF diagnostic is calibrated by producing a known amount of methyl through photo-dissociation of acetone vapor in a calibration gas mixture. We demonstrate PF-LIF imaging of methyl production in methane-containing nanosecond pulsed plasmas impinging on dielectric surfaces. Absolute calibration of the diagnostic is demonstrated in a diffuse, plane-to-plane discharge. Measured profiles show a relatively uniform distribution of up to 30 ppm of methyl. Relative methyl measurements in a filamentary plane-to-plane discharge and a plasma jet reveal highly localized intense production of methyl. The utility of the PF-LIF technique is further demonstrated by combining methyl measurements with formaldehyde LIF imaging to capture spatiotemporal correlations between methyl and formaldehyde, which is an important intermediate species in plasma-assisted oxidative coupling of methane.
In this LDRD project, we developed a versatile capability for high-resolution measurements of electron scattering processes in gas-phase molecules, such as ionization, dissociation, and electron attachment/detachment. This apparatus is designed to advance fundamental understanding of these processes and to inform predictions of plasmas associated with applications such as plasma-assisted combustion, neutron generation, re-entry vehicles, and arcing that are critical to national security. We use innovative coupling of electron-generation and electron-imaging techniques that leverages Sandia’s expertise in ion/electron imaging methods. Velocity map imaging provides a measure of the kinetic energies of electrons or ion products from electron scattering in an atomic or molecular beam. We designed, constructed, and tested the apparatus. Tests include dissociative electron attachment to O2 and SO2, as well as a new method for studying laser-initiated plasmas. This capability sets the stage for new studies in dynamics of electron scattering processes, including scattering from excited-state atoms and molecules.
This work describes the diagnostic implementation and image processing methods to quantitatively measure diesel spray mixing injected into a high-pressure, high-temperature environment. We used a high-repetition-rate pulse-burst laser developed in-house, a high-speed CMOS camera, and optimized the optical configuration to capture Rayleigh scattering images of the vaporized fuel jets inside a constant volume chamber. The experimental installation was modified to reduce reflections and flare levels to maximize the images’ signal-to-noise ratios by anti-reflection coatings on windows and surfaces, as well as series of optical baffles. Because of the specificities of the high-speed system, several image processing techniques had to be developed and implemented to provide quantitative fuel concentration measurements. These methods involve various correction procedures such as camera linearity, laser intensity fluctuation, dynamic background flare, as well as beam-steering effects. Image inpainting was also applied to correct the Rayleigh scattering signal from large scatterers (e.g. particulates). The experiments demonstrate that applying planar laser Rayleigh scattering at high repetition rate to quantitatively resolve the mixing of fuel and ambient gases in diesel jets is challenging, but possible. The thorough analysis of the experimental uncertainty and comparisons to past data prove that such measurements can be accurate, whilst providing valuable information about the mixing processes of high-pressure diesel jets.
Many important chemically reacting systems are inherently multi-dimensional with spatial and temporal variations in the thermochemical state, which can be strongly coupled to interactions with transport processes. Fundamental insights into these systems require multi-dimensional measurements of the thermochemical state as well as fluid dynamics quantities. Laser-based imaging diagnostics provide spatially and temporally resolved measurements that help address this need. The state of the art in imaging diagnostics is continually progressing with the goal of attaining simultaneous multi-parameter measurements that capture transient processes, particularly those that lead to stochastic events, such as localized extinction in turbulent combustion. Development efforts in imaging diagnostics benefit from advances in laser and detector technology. This article provides a perspective on the progression of increasing dimensionality of laser-based imaging diagnostics and highlights the evolution from single-point measurements to 1D and 2D multi-parameter imaging and 3D high-speed imaging. This evolution is demonstrated using highlights of laser-based imaging techniques in combustion science research as an exemplar of a complex multi-dimensional chemically reacting system with chemistry-transport coupling. Imaging diagnostics impact basic research in other chemically reacting systems as well, such as measurements of near-surface gases in heterogeneous catalysis. The expanding dimensionality of imaging diagnostics leads to larger and more complex datasets that require increasingly demanding approaches to data analysis and provide opportunities for increased collaboration between experimental and computational researchers in tackling these challenges.
High-speed, three-dimensional (3D) scalar-velocity field measurements were demonstrated in a lifted partially-premixed dimethyl-ether/air jet flame using simultaneous laser-induced fluorescence (LIF) of formaldehyde and tomographic particle image velocimetry (TPIV). The 3D LIF measurements were conducted by raster scanning the laser beam from a 100 kHz pulse-burst laser across the probe volume using an acousto-optic deflector. The volumetric reconstruction of the LIF signal from ten parallel planes provides quasi-instantaneous 3D LIF measurements that are synchronized with 10 kHz TPIV measurements. The temporally resolved formaldehyde-LIF and velocity field data were employed to analyze Lagrangian particle trajectories and displacement speeds at the base of the lifted flame. The particle trajectories revealed flow structures that are difficult to observe in an Eulerian reference frame. Positive and negative displacement speeds were observed at the formaldehyde-LIF surfaces at the inner and outer regions of the jet flame with a maximum displacement speed of approximately eight times the laminar flame speed of a stoichiometric dimethyl-ether/air mixture.
The effects of heat release on interactions between vorticity (ω) and strain rate (s) in turbulent premixed CH4/O2/N2 counterflow flames are investigated using simultaneous OH laser-induced fluorescence (LIF) and tomographic particle image velocimetry (TPIV) measurements. A comparison between the flames and a corresponding turbulent non-reacting variable density N2-vs-products counterflow reveals the impact of heat release on vorticity-strain rate alignment statistics. Vorticity and strain rate statistics in the flames and non-reacting flow are conditioned on distance from the local flame front and gas mixing layer interface (GMLI) contours, respectively. The magnitude, alignment, and spatial distribution of the vorticity and principal strain rates (s1, s2, s3) are rather different when heat release is present. Density variations without heat release enhance the ω-s2 alignment while significantly reducing the ω-s3 alignment and modestly reducing the ω-s1 alignment. In contrast, heat release at the flame front further reduces the ω-s1 alignment but increases the ω-s3 alignment and suppresses the preferential ω-s2 alignment. Furthermore, increasing turbulence diminishes the effect of heat release on this preferential alignment. In regions with the largest vorticities, both the reacting and non-reacting counterflows show an increase in the probability of ω-s2 alignment. All counterflow cases have a net positive vortex-stretching contribution to the enstrophy production with a peak production rate at the flame front or GMLI, but the peak values depend on the density variation, heat release, and turbulence level. Elucidation of the complex interplay between these factors contributes to the understanding of the dynamics of turbulence-flame interactions.
Fundamental chemistry in heterogeneous catalysis is increasingly explored using operando techniques in order to address the pressure gap between ultrahigh vacuum studies and practical operating pressures. Because most operando experiments focus on the surface and surface-bound species, there is a knowledge gap of the near-surface gas phase and the fundamental information the properties of this region convey about catalytic mechanisms. We demonstrate in situ visualization and measurement of gas-phase species and temperature distributions in operando catalysis experiments using complementary near-surface optical and mass spectrometry techniques. The partial oxidation of methanol over a silver catalyst demonstrates the value of these diagnostic techniques at 600 Torr (800 mbar) pressure and temperatures from 150 to 410 °C. Planar laser-induced fluorescence provides two-dimensional images of the formaldehyde product distribution that show the development of the boundary layer above the catalyst under different flow conditions. Raman scattering imaging provides measurements of a wide range of major species, such as methanol, oxygen, nitrogen, formaldehyde, and water vapor. Near-surface molecular beam mass spectrometry enables simultaneous detection of all species using a gas sampling probe. Detection of gas-phase free radicals, such as CH3 and CH3O, and of minor products, such as acetaldehyde, dimethyl ether, and methyl formate, provides insights into catalytic mechanisms of the partial oxidation of methanol. The combination of these techniques provides a detailed picture of the coupling between the gas phase and surface in heterogeneous catalysis and enables parametric studies under different operating conditions, which will enhance our ability to constrain microkinetic models of heterogeneous catalysis.
Abstract: Beam steering by index-of-refraction gradients poses a significant challenge for laser-based imaging measurements in turbulent reacting and non-reacting flows, particularly at elevated pressures. High fidelity imaging and quantitative data interpretation in turbulent flows can be considerably impeded by artefacts generated from beam steering. A wavelet-based filtering scheme has been developed to recover the underlying turbulent flow structures from imaging measurements containing severe beam-steering artefacts. This analysis technique is equally applicable to imaging measurements in reacting and non-reacting flows. It is demonstrated using mixture fraction measurements in a transient turbulent jet flow at 8 bar using Rayleigh scattering imaging at a repetition rate of 100 kHz. The corrected images reveal the temporal evolution of flow structures with negligible residual beam-steering artefacts. Tests of the sensitivity of the wavelet-based filtering scheme to noise and spatial resolution indicate that it is a robust analytic tool for correcting severe beam-steering artefacts commonly encountered in laser-based imaging measurements at elevated pressures. Graphic abstract: [Figure not available: see fulltext.].
This project explored a new capability for studying collisions of electrons and molecules with unprecedented accuracy by combining high electron-energy resolution with velocity mapped imaging of electrons. Low-energy electrons were produced within a supersonic beam by photoionization of metastable krypton using a dye laser to generate electrons with tunable kinetic energy and a narrow energy spread. A new configuration for electron imaging optics was developed to enable scattering of electrons in a zero-field environment with subsequent rapidly pulsed velocity mapped imaging of the electrons. Development of this new capability will significantly enhance DOE/NNSA's ability to perform basic research on processes relevant to plasmas in atmospheric re-entry and neutron generation for weapons systems and provide fundamental understanding of electron-driven chemistry important to solar energy conversion.