Nature of the magnetic excitation spectrum in (Sm,Y)S: CEF effects or an exciton?

The dynamic magnetic susceptibility spectrum in a single-crystal sample of the intermediate-valence compound Sm_0.67Y_0.33S is studied by inelastic neutron scattering with neutron momentum transfer and sample temperatures varying over wide ranges. Two coupled collective modes have been found in the spectrum. Unlike the higher energy mode, whose intensity approximately follows the form factor of Sm²⁺, the lower energy mode exhibits a stronger angular dependence than could be expected from the form factor for the localized f electrons. The total intensity of the inelastic component of the magnetic response decreases with increasing temperature; this is accompanied by the appearance of a broad quasi-elastic signal of a magnetic nature at significantly lower temperatures than follows from the calculated intensities of the transitions within the excited multiplet of the Sm²⁺ ion. An analysis of the observed features allows the suggestion to be made that the fine structure of the magnetic excitation spectrum in (Sm,Y)S is associated with the formation of an exciton-like intermediate-valence state on Sm ions rather than with the crystal-electric-field effects.