Quasielastic neutron scattering experiments and molecular dynamics (MD) simulations have been used to investigate molecular diffusive motion near the melting transition of monolayers of flexible rod-shaped molecules. The experiments were conducted on butane and hexane monolayers adsorbed on an exfoliated graphite substrate, For butane, quasielastic scattering broader than the experimental energy resolution width of 70 mu eV appears abruptly at the monolayer melting point of T-m = 116 K, whereas, for the hexane monolayer, it appears 20 K below the melting transition (T-m = 170 K). To facilitate comparison with experiment, quasielastic spectra calculated from the MD simulations were analyzed using the same models and fitting algorithms as for the neutron spectra. This combination of techniques gives a microscopic picture of the melting process in these two monolayers which is consistent with earlier neutron diffraction experiments. Butane melts abruptly to a liquid phase where the molecules in the trans conformation translationally diffuse while rotating about their center of mass. In the case of the hexane monolayer, the MD simulations show that the appearance of quasielastic scattering below T-m coincides with transformation of Some molecules from trans to gauche conformations. Furthermore, if gauche molecules are prevented from forming in the simulation, the calculated incoherent scattering function contains no quasielastic component below T-m. Modeling of both the neutron and simulated hexane monolayer spectra below T-m favors a plastic phase in which there is nearly isotropic rotational diffusion of the gauche molecules about their center of mass, but no translational diffusion, The elastic scattering observed above T-m is consistent with the coexistence of solid monolayer clusters with a fluid phase, as predicted by the simulations. For T/T-m greater than or equal to 1.3, the elastic scattering vanishes from the neutron spectra where the simulation indicates the presence of a fluid phase alone, The qualitative similarities between the observed and simulated quasielastic spectra lend support to a previously proposed ''footprint reduction'' mechanism of melting in monolayers of flexible, rod-shaped molecules. (C) 1997 American Institute of Physics.