Quantitative CARS spectroscopy of CO2 and N2O

Experimental and theoretical investigations of the CARS spectroscopy of CO2(2v2) and N2O(v3) were carried out. The experimental spectra were measured in a heated test cell, and excellent agreement with the observed temperature dependences was obtained from numerical simulations. Assignments were made for all hot bands, and the role of collisional narrowing was quantified. Observed nonresonant susceptibility effects in pure N2O have made it possible to estimate the nonresonant background susceptibility for this molecule by using the resonant contribution as a reference calibration.