Using time-resolved polarization spectroscopy we have observed quantum
beats of coherently excited states in the (A(2) Sigma(+)-X(2) Pi) vib
ronic (0, 0) band system of OH in atmospheric-pressure flames. With a
spectral bandwidth of 1 cm(-1) of the tunable coherent light source em
ployed, line splittings were deduced from the temporal beat structure.
Depending on the rotational quantum number of the probed transition a
nd the collisional environment the relaxation times of anisotropic ori
entational distributions in which the quantum beat oscillations were o
bserved ranged between 120 ps (J '' = 5) and 368 ps (J '' = 10).