Publications

Coherent anti-Stokes Raman scattering (CARS) is commonly used for thermometry and concentration measurement of major species. The quadratic scaling of CARS signal with number density has limited the use of CARS for detection of minor species, where more sensitive approaches may be more attractive. However, significant advancements in ultrafast CARS approaches have been made over the past two decades, including the development of hybrid CARS demonstrated to yield greatly increased excitation efficiencies. Yet, detailed detection limits of hybrid CARS have not been well established. In this Letter, detection limits for N2, H2, CO, and C2H4 by point-wise hybrid femtosecond (fs)/picosecond (ps) CARS are determined to be of the order of 1015 molecules/cm3. The possible benefit of fs/nanosecond (ns) hybrid CARS is also discussed.

The role of a solid surface for initiating gas-phase reactions is still not well understood. The hydrogen atom (H) is an important intermediate in gas-phase ethane dehydrogenation and is known to interact with surface sites on catalysts. However, direct measurements of H near catalytic surfaces have not yet been reported. Here, we present the first H measurements by laser-induced fluorescence in the gas-phase above catalytic and noncatalytic surfaces. Measurements at temperatures up to 700 °C show H concentrations to be at the highest above inert quartz surfaces compared to stainless steel and a platinum-based catalyst. Additionally, H concentrations above the catalyst decreased rapidly with time on stream. These newly obtained observations are consistent with the recently reported differences in bulk ethane dehydrogenation reactivity of these materials, suggesting H may be a good reporter for dehydrogenation activity.

Coherent anti-Stokes Raman scattering (CARS) is a valuable spectroscopic tool for the measurement of temperature and species concentration. In recent years, multi-dimensional CARS has seen focused development and is especially important in reacting flows. An important aspect of multi-dimensional CARS is the phase-matching scheme used. Historically, collinear and BOXCARS phase-matching schemes have been used to achieve phase matching over a broad spectral range. For 1-D and 2-D CARS imaging, two-beam or counter-propagating beam arrangements are necessary. The two-beam arrangement offers many advantages, but introduces a phase mismatch which limits the spectral response of the measurement. This work explores the tradeoffs in spatial resolution, spectral bandwidth, and CARS intensity in 2-D CARS arrangements. Calculations are made for two-beam and counter-propagating beam CARS.