The firstCARS measurements of temperature and species concentrations in the exhaust of solid propellants burning at elevated pressure (≤ 35 atm) are reported. Multiple species data are acquired at high temporal (10 ns) and spatial resolution from both a homogeneous, double-base and a composite nitramine propellant. CARS spectra have been obtained from three spectral regions that encompass the signatures of the major combustion products, CO2, CO-N2,and H2O. The CARS data are analyzed by comparison with computer synthesized spectra generated at various temperatures and species concentrations. Results in the postflame zone from nitramine combustion at 23 atm indicate temperatures as high as 2600 K with species concentrations of N2 ∼ 23%, CO ∼ 36%, and H2 ∼ 23%. These results compare favorably with predictions of temperature and concentration from a chemical equilibrium code that simulates the combustion parameters. Utilization of dual broadband approaches will allow the simultaneous acquisition of data from ...