Ferroquadrupole ordering and Γ5 rattling motion in the clathrate compound Ce3Pd20Ge6 -: art. no. 184109

Lattice effects in a cerium based clathrate compound Ce3Pd20Ge6 with a cubic Cr23C6-type structure have been investigated by ultrasonic and thermal expansion measurements. Elastic softenings of (C-11-C-12)/2 and C-44 proportional to the reciprocal temperature 1/T above T-Q1=1.25 K are well described in terms of the quadrupole susceptibility for the ground state Gamma(8) quartet. A huge softening of 50% in (C-11-C-12)/2 and a spontaneous expansion DeltaL/L=1.9x10(-4) along the [001] direction in particular indicate the ferroquadrupole ordering of O-2(0) below T-Q1. The elastic anomalies associated with the antiferromagnetic ordering at T-N2=0.75 K and the incommensurate antiferromagnetic ordering are also found. Notable frequency dependence of C-44 around 10 K is accounted for by the Debye-type dispersion indicating a Gamma(5) rattling motion of an off-center Ce ion along the [111] direction with eight fractionally occupied positions around the 4a site in a cage. The thermally activated Gamma(5) rattling motion obeying a relaxation time tau=tau(0) exp (E/k(B)T) with an attempt time tau(0)=3.1x10(-11) sec and an activation energy E=70 K dies out with decreasing temperature, and then the off-center tunneling state of Ce ion in the 4a-site cage will appear at low temperatures.