Publications

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We report the application of ultrafast rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning aluminized ammonium perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laserbased diagnostics, with intense background luminosity, scattering and beam obstruction from hot metal particles that can be as large as several hundred microns in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminumparticle- seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulateenhanced laser-induced breakdown. Introduction of fs/ps laser pulses enables CARS detection at reduced pulse energies, decreasing the likelihood of breakdown, while simultaneously providing time-gated elimination of any nonresonant background interference. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements from the fs/ps rotational CARS measurement volume positioned within 3 mm or less of the burning propellant surface. Preliminary results in canonical flames are presented using a hybrid fs/ps vibrational CARS system to demonstrate our progress towards acquiring vibrational CARS measurements for more accurate temperatures in the very high temperature propellant burns.

While historically there have been many demonstrations of phase-conjugate holography to correct for noise created by phase distortions, the technique has not been applied to modern digital inline holographic measurements. Here, we present the theory and initial experiments exploring the impact of using phase-conjugate digital inline holography (PCDIH) to reduce noise produced by phase distortions through index-of-refraction gradients, such as would be experienced in a combustion environment. We demonstrate the ability to measure 3D object locations using PCDIH and correct for some types of disturbances. To quantify the technique, a plasma generator is used to produce strong indexof- refraction changes in room air. Object position errors in these measurements from both traditional DIH and PCDIH are compared. Preliminary results suggest that the use of PCDIH could potentially reduce positional error by approximately half when measuring through phase disturbances.

We report the application of ultrafast rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning aluminized ammonium perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laserbased diagnostics, with intense background luminosity, scattering and beam obstruction from hot metal particles that can be as large as several hundred microns in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminumparticle- seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulateenhanced laser-induced breakdown. Introduction of fs/ps laser pulses enables CARS detection at reduced pulse energies, decreasing the likelihood of breakdown, while simultaneously providing time-gated elimination of any nonresonant background interference. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements from the fs/ps rotational CARS measurement volume positioned within 3 mm or less of the burning propellant surface. Preliminary results in canonical flames are presented using a hybrid fs/ps vibrational CARS system to demonstrate our progress towards acquiring vibrational CARS measurements for more accurate temperatures in the very high temperature propellant burns.

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The interaction of a Mach 1.67 shock wave with a dense particle curtain is quantified using flash radiography. These new data provide a view of particle transport inside a compressible, dense gas–solid flow of high optical opacity. The curtain, composed of 115-µm glass spheres, initially spans 87 % of the test section width and has a streamwise thickness of about 2 mm. Radiograph intensities are converted to particle volume fraction distributions using the Beer–Lambert law. The mass in the particle curtain, as determined from the X-ray data, is in reasonable agreement with that given from a simpler method using a load cell and particle imaging. Following shock impingement, the curtain propagates downstream and the peak volume fraction decreases from about 23 to about 4 % over a time of 340 µs. The propagation occurs asymmetrically, with the downstream side of the particle curtain experiencing a greater volume fraction gradient than the upstream side, attributable to the dependence of particle drag on volume fraction. Bulk particle transport is quantified from the time-dependent center of mass of the curtain. The bulk acceleration of the curtain is shown to be greater than that predicted for a single 115-µm particle in a Mach 1.67 shock-induced flow.

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We present a detailed set of measurements from a piloted, sooting, turbulent C ₂ H ₄ - fueled diffusion flame. Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (CARS) is used to monitor temperature and oxygen, while laser-induced incandescence (LII) is applied for imaging of the soot volume fraction in the challenging jet-flame environment at Reynolds number, Re = 20,000. Single-laser shot results are used to map the mean and rms statistics, as well as probability densities. LII data from the soot-growth region of the flame are used to benchmark the soot source term for one-dimensional turbulence (ODT) modeling of this turbulent flame. The ODT code is then used to predict temperature and oxygen fluctuations higher in the soot oxidation region higher in the flame.

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We report measurements of temperature and O2/N2 mole-fraction ratio in the vicinity of a burning and decomposing carbon-epoxy composite aircraft material samples exposed to uniform heat fluxes of 48 and 69 kW/m2. Controlled laboratory experiments were conducted with the samples suspended above a cone-type heater and enclosed in an optically accessible chimney. Noninvasive coherent anti-Stokes Raman scattering (CARS) measurements we performed on a single-laser-shot basis. The CARS data were performed with both a traditional point measurement system and with a one-dimensional line imaging scheme that provides single-shot temperature and O2/N2 profiles to reveal the quantitative structure of the temperature and oxygen concentration profiles over the duration of the 30-40 minute duration events. The measured near-surface temperature and oxygen transport are an important factor for exothermic chemistry and oxidation of char materials and the carbon fibers themselves in a fire scenario. These unique laser-diagnostic experiments provide new information on physical/chemical processes in a well-controlled environment which may be useful for the development of heat-and mass-transfer models for the composite fire scenario.

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We present the results of an LDRD project to develop diagnostics to perform fundamental measurements of material properties during shock compression of condensed phase materials at micron spatial scales and picosecond time scales. The report is structured into three main chapters, which each focus on a different diagnostic devel opment effort. Direct picosecond laser drive is used to introduce shock waves into thin films of energetic and inert materials. The resulting laser - driven shock properties are probed via Ultrafast Time Domain Interferometry (UTDI), which can additionally be used to generate shock Hugoniot data in tabletop experiments. Stimulated Raman scattering (SRS) is developed as a temperature diagnostic. A transient absorption spectroscopy setup has been developed to probe shock - induced changes during shock compressio n. UTDI results are presented under dynamic, direct - laser - drive conditions and shock Hugoniots are estimated for inert polystyrene samples and for the explosive hexanitroazobenzene, with results from both Sandia and Lawrence Livermore presented here. SRS a nd transient absorption diagnostics are demonstrated on static thin - film samples, and paths forward to dynamic experiments are presented.

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A simple spectral focusing scheme for bandwidth optimization of gas-phase rotational coherent anti- Stokes Raman scattering (CARS) spectra is presented. The method is useful when femtosecond pump/Stokes preparation of the Raman coherence is utilized. The approach is of practical utility when working with laser pulses that are not strictly transform limited or when windows or other sources of pulse chirp may be present in the experiment. A delay between the femtosecond preparation pulses is introduced to shift the maximumRaman preparation away from zero frequency and toward the Stokes or anti-Stokes side of the spectrum with no loss in total preparation bandwidth. Shifts of 100 cm-1or more are attainable and allow for enhanced detection of high-energy (150-300 cm-1) rotational Raman transitions at near-transform-limited optimum sensitivity. A simple theoretical treatment for the case of identical pump and Stokes pulses with linear frequency chirp is presented. The approach is then demonstrated experimentally for typical levels of transform-limited laser performance obtained in our laboratory with nonresonant CARS in argon and Raman-resonant spectra from a lean H2/air flat flame.

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A hybrid fs/ps pure-rotational coherent anti-Stokes Raman scattering (CARS) scheme is systematically evaluated over a wide range of flame conditions in the product gases of two canonical flat-flame burners. Near-transform-limited, broadband femtosecond pump and Stokes pulses impulsively prepare a rotational Raman coherence, which is later probed using a high-energy, frequency-narrow picosecond beam generated by the second-harmonic bandwidth compression scheme that has recently been demonstrated for rotational CARS generation in H2/air flat flames. The measured spectra are free of collision effects and nonresonant background and can be obtained on a single-shot basis at 1kHz. The technique is evaluated for temperature/oxygen measurements in near-adiabatic H2/air flames stabilized on the Hencken burner for equivalence ratios of ϕ=0.20-1.20. Thermometry is demonstrated in hydrocarbon/air products for ϕ=0.75-3.14 in premixed C2H4/air flat flames on the McKenna burner. Reliable spectral fitting is demonstrated for both shot-averaged and single-laser-shot data using a simple phenomenological model. Measurement accuracy is benchmarked by comparison to adiabatic-equilibrium calculations for the H2/air flames, and by comparison with nanosecond CARS measurements for the C2H4/air flames. Quantitative accuracy comparable to nanosecond rotational CARS measurements is observed, while the observed precision in both the temperature and oxygen data is extraordinarily high, exceeding nanosecond CARS, and on par with the best published thermometric precision by femtosecond vibrational CARS in flames, and rotational femtosecond CARS at low temperature. Threshold levels of signal-to-noise ratio to achieve 1-2% precision in temperature and O2/N2 ratio are identified. The results show that pure-rotational fs/ps CARS is a robust and quantitative tool when applied across a wide range of flame conditions spanning lean H2/air combustion to fuel-rich sooting hydrocarbon flames.

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We present the results of a two year early career LDRD project, which has focused on the development of ultrafast diagnostics to measure temperature, pressure and chemical change during the shock initiation of energetic materials. We compare two single-shot versions of femtosecond rotational CARS to measure nitrogen temperature: chirped-probe-pulse and ps/fs hybrid CARS thermometry. The applicability of measurements to the combustion of energetic materials will be discussed. We have also demonstrated laser shock and particle velocity measurements in thin film explosives using stretched femtosecond laser pulses. We will discuss preliminary results from Al and PETN thin films. Agreement between our results and previous work will be discussed.

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