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It has recently been shown that relaxation of the rotational energy of hotnon-equlibrium photofragments (i) slows down significantly with the increase oftheir initial rotational temperature and (ii) differs dramatically from therelaxation of the equilibrium rotational energy correlation function,manifesting thereby breakdown of the linear response description [Science 311,1907 (2006)]. We demonstrate that this phenomenon may be caused by the angularmomentum dependence of rotational friction. We have developed the generalizedFokker-Planck equation whose rotational friction depends upon angular momentumalgebraically. The calculated rotational correlation functions correspond wellto their counterparts obtained via molecular dynamics simulations in a broadrange of initial non-equilibrium conditions. It is suggested that the angularmomentum dependence of friction should be taken into account while describingrotational relaxation far from equilibrium

Angular momentum dependent friction slows down rotational relaxation under nonequilibrium conditions