We present polarized two-photon excitation (TPE) spectra for samarium(III)
f(5) in the elpasolite Cs2NaYCI6. Approximately 80 levels have been assigne
d up to 29 000 cm(-1) with the aid of a one-electron crystal field Hamilton
ian, representing the most complete and extensive data set so far reported
for Sm(III) at a cubic site. Deviations from the predictions of one-electro
n theory are discussed in terms of the spin correlated crystal held (SCCF).