Coherent anti-Stokes Raman scattering (CARS) spectra of HCl, N-2, and
the nu(1) fundamental of C2H2 have been measured in the gas phase. The
measured spectra show rotational structures which originate from the
Q-branch transitions. The spectra have successfully been simulated wit
h proper selection rules, line positions, and relative intensities fro
m room temperature Boltzmann population distributions. The vibration-r
otation interaction constant alpha of HCl in the ground electronic sta
te has been measured from the rotationally resolved CARS spectra which
is alpha=0.3076 cm(-1). Possibilities of optical pumping and of measu
ring state specific energy distributions of molecules are discussed.