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Using a combination of velocity-map imaging and resonance-enhanced multiphoton ionization detection with crossed molecular beam scattering, the dynamics of rotational energy transfer have been examined for NO in collisions with CH 4 at a mean collision energy of 700 cm  - 1 . The images of NO scattered into individual rotational ( j  NO  ' ) and spin-orbit (Ω) levels typically exhibit a single broad maximum that gradually shifts from the forward to the backward scattering direction with increasing rotational excitation (i.e., larger Δ j  NO ). The rotational rainbow angles calculated with a two-dimensional hard ellipse model show reasonable agreement with the observed angles corresponding to the maxima in the differential cross sections extracted from the images for higher Δ j  NO ransitions, but there are clear discrepancies for lower Δ j  NO (in particular, final rotational levels with j  NO  ' = 7.5 and 8.5). The sharply forward scattered angular distributions for these lower Δ j  NO ransitions better agree with the predictions of an L-type rainbow model. The more highly rotationally excited NO appears to coincide with low rotational excitation of the co-product CH 4 , indicating a degree of rotational product-pair anticorrelation in this bimolecular scattering.

Observation of Rainbows in the Rotationally Inelastic Scattering of NO with CH4

Observation of Rainbows in the Rotationally Inelastic Scattering of NO with CH₄