<p dir="ltr">This dissertation describes efforts in the development of an optically-accessible solid fuel ramjet combustion experiment and the application, and requisite modifications, of multiple laser-based diagnostics. These measurements target the characterization of the complex turbulent reacting flow physics in a multi-phase combustion environment representative of conditions within a solid fuel ramjet.</p><p dir="ltr"><br>First, dynamic flow-flame interactions were investigated in an optically-accessible solid fuel ramjet combustor. Experiments were performed with a single hydroxyl-terminated polybutadiene fuel slab located downstream of a backward-facing step in a rectangular chamber. To emulate flight-relevant combustor conditions, unvitiated heated air was directed through the combustion chamber with an inlet temperature of ∼655 K, chamber pressures of 450–690 kPa, and port Reynolds number of ∼500,000. 20 kHz OH∗-chemiluminescence and 10 kHz particle imaging velocimetry measurements were used to characterize the heat-release distribution and velocity field. Comparison between the mean OH∗ chemiluminescence images acquired at three flow conditions indicates reduction in flame height above the grain with increasing air mass flow rate. Dominant heat-release coherent structures in the statistically stationary flow are identified using the spectral proper orthogonal decomposition technique implemented on time-series of instantaneous images. The spatial mode shapes of the chemiluminescence and velocity field measurements indicated that the flow-flame interactions were dominated by vortex shedding generated at the backward facing step in the combustor, at Strouhal numbers of 0.06 – 0.10.</p><p dir="ltr"><br>Following this effort, a coherent anti-Stokes Raman scattering (CARS) laser system was assembled and aligned for measurements of the Q-branch ro-vibrational energy level structure of nitrogen using a coannular phase-matching scheme and frequency-shifted probe beam. These measurements were demonstrated in the model SFRJ combustion chamber operated with an inlet air temperature of 690 K and pressure of 0.59 MPa. Over 300 single-shot spectra were collected and fit for temperatures ranging from the core air flow to the combustion gases with a probe location situated above the redeveloping boundary layer region diffusion flame. A skewed temperature distribution was reported at the probe location, as expected from a region only intermittently exposed to hot combustion gases. Temperatures of 500-2000 K were fit to theory, indicating a requirement for high dynamic range measurements.</p><p dir="ltr"><br>A handful of shortcomings were identified in the application of the shifted-CARS technique to the luminous SFRJ flow-field and thus modifications were made to the CARS system for improved dynamic range, signal-to-noise ratio and signal-to-interference ratio. A dual-pump system provided simultaneous measurements of the Q-branch ro-vibrational energy level structure of nitrogen and pure-rotational energy level structure of nitrogen and oxygen. These spectra possessed ample features for accurate comparison to theory at temperatures of 600-2500 K, a typical range at flame locations within the highly dynamic SFRJ reacting flow. Additionally, an electro-optical shutter (EOS), comprised of a Pockels cell located between crossed-axis polarizers, was integrated into the CARS system. The use of the EOS enabled thermometry measurements in high luminosity flames through significant reduction of the background resulting from broadband flame emission. Temporal gating ≤100 nanoseconds along with an extinction ratio >10,000:1 was achieved using the EOS. Integration of the EOS enabled the use of an unintensified CCD camera for signal detection, improving upon the signal-to-noise ratio achievable with inherently noisy microchannel plate intensification processes, previously employed for short temporal gating.<br></p><p dir="ltr">Using this system, temperature and relative oxygen concentration scalar fields were measured in an optically accessible solid fuel ramjet (SFRJ) combustion chamber using coherent anti-Stokes Raman scattering (CARS). Additionally, planar laser-induced fluorescence measurements of the hydroxyl radical (OH-PLIF) were performed to spatially characterize flame location and provide context to the temperature measurements. The combustion chamber was operated with an inlet air temperature of 670 K, mass flowrate of 1.14 kg/s, and pressure of 0.57 MPa, conditions relevant to practical device operation. The dual-pump CARS system provided simultaneous measurements of the Q-branch ro-vibrational energy level structure of nitrogen and pure-rotational energy level structure of nitrogen and oxygen. These spectra possessed ample features for accurate comparison to theory at temperatures of 600-2500 K, a typical range at flame locations within the highly dynamic SFRJ reacting flow<br>and inherently track the relative oxygen concentration within the measurement volume. A skewed temperature distribution was reported at various probe locations, as expected from stochastic probing of dynamic reacting vortex structures. Comparison between CARS and OH-PLIF measurements within the flow impingement region indicated that the high temperature regions closely align with regions of high OH-PLIF intensity while the temperature standard deviation better matches the flame-surface density. The signal intensity distribution within instantaneous OH-PLIF images indicates transport of combustion products toward the grain, supported by the near-wall peak temperatures. This process is critical for the transport of energy to the grain such that additional fuel can be volatilized and mix with the air to support the flame.</p><p dir="ltr"><br>Finally, an ultra-fast CARS system has been designed and aligned for 1 kHz one-dimensional measurements of temperature by targeting the ro-vibrational Q-branch transitions of nitrogen. This effort seeks to develop a technique that can capture the hydrodynamics that drive the combustion in SFRJ and provide an intuition for the energy transport near the solid fuel wall of the SFRJ combustor through capturing instantaneous temperature profiles. The designed system utilized a 9 W high-energy regenerative amplifier with 30 fs duration pulses.<br>For the CARS measurement, the 4 W 800 nm output from the external compressor is used as the Stokes beam and a 0.5 W, 675 nm ouput from the TOPAS optical parametric amplifier (OPA) split to and used as the pump and probe beams. A chirping rod placed in the beam path of the probe beam was used to generate the picosecond pulse. Preliminary measurements have been acquired within room air and a laminar H2-Air nonpremixed flame. A discussion of the experimental challenges and remaining work is presented in this document.</p>