An aligned sample of HD(v = 1, J = 2, MJ = 0) molecules is prepared under collision-free conditions using the S(0) stimulated Raman pumping transition. Subsequent coupling to the spins of the deuteronID and the proton IH causes the initial degree of alignment to oscillate and decrease as monitored over the time range from 0–13 μs via the O(2) line of the [2 + 1] REMPIE,F1Σ+g−X1Σ+g (0,1) band. The time dependence of the rotational alignment is also calculated using both a hierarchical coupling scheme in which the rotational angular momentum J is regarded first to couple to ID, and then the resultant Fi to couple to IH, to form the total angular momentum F and a non-hierarchical coupling scheme in which the HD energy level structure is not assumed to be diagonal in the |IH(JID)FiFMF> basis set. The experimental data is in good agreement with the non-hierarchical calculation but not with the hierarchical calculation, as expected for this system. Additionally, we calculate the time dependence of the H and D nuclear spin polarizations.
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