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Time-domain self-broadened and air-broadened nitrogen S-branch Raman linewidths at 80-200 K recorded in an underexpanded jet

Journal of Chemical Physics

Richardson, Daniel R.; Retter, Jonathan E.; Koll, Matthew K.; Kearney, S.P.

We report pure-rotational N2-N2, N2-air, and O2-air S-branch linewidths for temperatures of 80-200 K by measuring the time-dependent decay of rotational Raman coherences in an isentropic free-jet expansion from a sonic nozzle. We recorded pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) spectra along the axial centerline of the underexpanded jet, within the barrel shock region upstream of the Mach disk. The dephasing of the pure-rotational Raman coherence was monitored using probe-time-delay scans at different axial positions in the jet, corresponding to varying local temperatures and pressures. The local temperature was obtained by fitting CARS spectra acquired at zero probe time delay, where the impact of collisions was minimal. The measured decay of each available Raman transition was fit to a dephasing constant and corrected for the local pressure, which was obtained from the CARS-measured static temperature and thermodynamic relationships for isentropic expansion from the known stagnation state. Nitrogen self-broadened transitions decayed more rapidly than those broadened in air for all temperatures, corresponding to higher Raman linewidths. In general, the measured S-branch linewidths deviated significantly in absolute and relative magnitudes from those predicted by extrapolating the modified exponential gap model to low temperatures. The temperature dependence of the Raman linewidth for each measured rotational state of nitrogen (J ≤ 10) and oxygen (N ≤ 11) was fit to a temperature-dependent power law over the measurable temperature domain (80-200 K) and extrapolated to both higher rotational states and room temperature. The measured and modeled low-temperature linewidth data provided here will aid low temperature gas-phase pressure measurements with fs/ps CARS.

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Laser-Diagnostic Platform for Multi-Parameter Hypersonics Measurements

Kearney, S.P.; Retter, Jonathan E.; Richardson, Daniel R.; Koll, Matthew K.

We have investigated the utility of femtosecond/picosecond (fs/ps) coherent anti-Stokes Raman scattering(CARS)for simultaneous measurement of temperature, pressure, and velocity in hypersonic flows. Experiments were conducted in underexpanded jets of air and molecular nitrogen to assess CARS diagnostic performance in terms of signal level scaling, measurement precision, and dynamic range. Pure-rotational CARS of the Raman S branch was applied for simultaneous measurement of temperature and pressure. Thermometry was performed by fitting CARS spectra acquired under nearly collision-free conditions by introducing a picosecond CARS probe pulse at zero delay from the femtosecond pump. Pressure could be subsequently obtained by from a second CARS spectral acquisition with a picosecond probe introduced at time delay to sample molecular collisions. CARS velocimetry was attempted by monitoring the Doppler shift of the N2 vibrational, Q-branch spectrum, with both direct spectral resolution and optical heterodyne detection schemes. Doppler shifts from the sub-I-km/s air jet flow proved too small to measure with this approach, prompting us to turn to femtosecond laser electronic excitation tagging (FLEET) for reliable single-laser-shot velocimetry and CARS temperature/pressure measurement. Scaling of the CARS signal level to very low pressure and temperature conditions expected in the Sandia hypersonic wind tunnel (HWI) was performed. CARS measurements of temperature in HWT appear to be very feasible, while prospects for HWT pressure measurements are reasonable.

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3 Results
3 Results