The valence state of Mn in magnetoresistive perovskites has been widely rel
ated to the level of alkaline metal substitution of the rare earth, by assu
ming that the Mn exists in 3 + or 4+ valence states. Measurements have been
made on a series of samples in the system Pr1-(x+y)(CaxSryMnO3. Mn-55 nucl
ear magnetic resonance (NMR) zero field spin echo measurements on a single
crystal with x=0.1 and y = 0 show distinct resonances around 310 MHz (Mn4+)
and 400 MHz (Mn3+) but also at 590 MHz (Mn2+). An increase in the Mn2+ res
onance frequency in an applied field implies that the Mn2+ moment is antife
rromagnetically coupled to the net magnetization. Spectra from powder sampl
es are much broader. The resonance frequencies increase as the Pr content i
s reduced. For systems with x + y = 0.4, there is little change in the NMP
spectrum as the proportions of Ca and Sr are altered. (C) 1998 American Ins
titute of Physics. [S0021-8979(98)26511-X].