  Synthesis and crystal structures are described for the compounds
Ln2(Ti2-xLnx)O7-x/2, where Ln = Tb, Dy, Ho, Er, Tm, Yb, Lu, and x ranges from 0
to 0.67. Rietveld refinements on X-ray powder diffraction data indicate that in
Tb and Dy titanate pyrochlores, extra Ln3+ cations mix mainly on the Ti4+ site
with little disorder on the original Ln3+ site. For the smaller rare earths
(Ho-Lu), stuffing additional lanthanide ions results in a pyrochlore to defect
fluorite transition, where the Ln3+ and Ti4+ ions become completely randomized
at the maximum (x=0.67). In all of these Ln-Ti-O pyrochlores, the addition of
magnetic Ln3+ in place of nonmagnetic Ti4+ adds edge sharing tetrahedral spin
interactions to a normally corner sharing tetrahedral network of spins. The
increase in spin connectivity in this family of solid solutions represents a
new avenue for investigating geometrical magnetic frustration in the rare earth
titanate pyrochlores.
