Abstract

Time-resolved picosecond pump-probe polarization and degenerate four wave mixing (DFWM) spectroscopy have been applied for the observation of coherently excited states in the (0,0) band of the electronic A 2ΣX 2Π transition of OH in atmospheric pressure CH 4 air and H 2 O 2 flames. From the exponential decays of the signal after excitation with a 20 ps pump pulse the decay of orientation and alignment through dephasing collisions and rotational energy transfer takes place within 150–370 ps depending on the rotational state quantum number. For simultaneously excited transitions within the bandwidth of the picosecond laser pulse, oscillations in the transient DFWM signal superimposed on the exponential decay have been observed for cross-polarized pump and probe laser beams.

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