The pulsed-neutron experiment fundamental mode discrete time-decay constant has been calculated as a function of system size for spherical light water assemblies using realistic H2O scattering models by the discrete-ordinates method. Comparison with experiment shows agreement to be good. The computed energy spectra and angular distributions of the fundamental mode neutron fluxes are discussed and physical interpretations of their behavior are proffered. The effect of including various orders of anisotropy in the scattering kernel is examined. Decay-constant calculations were also performed for a model that neglects chemical binding. The results are compared with those based on models that include binding (and are in good agreement with experiment). The effects of chemical binding in neutron thermalization are shown to be significant by this comparison.