Observations of Dicke narrowing and speed dependence in air-broadened CO₂ lineshapes near 2.06 μm.

Abstract

Frequency-stabilized cavity ring-down spectroscopy was used to study CO2 lineshapes in the (20013) ← (00001) band centered near 2.06 μm. Two rovibrational transitions were chosen for this study to measure non-Voigt collisional effects for air-broadened lines over the pressure range of 7 kPa-28 kPa. Lineshape analysis for both lines revealed evidence of simultaneous Dicke (collisional) narrowing and speed-dependent effects that would introduce biases exceeding 2% in the retrieved air-broadening parameters if not incorporated in the modeling of CO2 lineshapes. Additionally, correlations between velocity- and phase/state changing collisions greatly reduced the observed Dicke narrowing effect. As a result, it was concluded that the most appropriate line profile for modeling CO2 lineshapes near 2.06 μm was the correlated speed-dependent Nelkin-Ghatak profile, which includes all of the physical effects mentioned above and leads to a consistent set of line shape parameters that are linear with gas pressure.