We have microscopically elucidated low-energy fluctuations in the completely filled skutterudites YbFe4Sb12 and LaFe4Sb12 through 121 Sb nuclear quadrupole resonance and 139 La nuclear magnetic resonance measurements. It provides evidence that upon cooling, YbFe4Sb12 transforms into a nonmagnetic heavy Fermi liquid state and LaFe4Sb12 remains the paramagnetic one, in contrast to the ferromagnetically ordered state and the heavy Fermi liquid-like one previously reported for the corresponding skutterudites with rare-earth deficiencies of about 10%. The local maxima in the longitudinal spin-lattice relaxation rate 1/T1 and transversal spin-spin relaxation rate 1/T2 for both LaFe4Sb12 and YbFe4Sb12 are ascribed to the freezing of thermal motions of rare-earth ion in each Sb-cage. It is suggested that the thermal motion of La ion (f 0 ) is of incoherent motion, whereas that of Yb ion (f 13 ) is of coherent one originating from possible interactions between f electrons in neighboring cages. It is also suggested that the coherent motion in YbFe4Sb12 is largely disturbed with increasing the extent of Yb-deficiency.
KEYWORDS: YbFe4Sb12, LaFe4Sb12, low energy fluctuations, NQR, NMRThe intriguing properties of filled skutterdites, such as heavy fermion superconductivity, metal-insulator transition and multipolar ordering, have attracted comprehensive studies, and much of the fundamental nature stemmed from the peculiar crystal structure have been clarified.1 The filled skutterudites with a formula RT 4 X 12 have a structure of space group Im3, in which rare-earth atom R is filled as a guest in each cage formed by twelve ligand pnictogen atoms X which allows the 4f electrons to move by mixing with neighboring p electron orbits, giving rise to the wide variety of strongly correlated electron phenomena. Possible contribution on the physical properties from the thermal fluctuations of R in each cage has also attracted intensive interest. However, some of experimental studies suggest that the physical properties are largely affected by the existence of rare-earth atom deficiency in the material. One of the important issues being left unsolved in filled skutterudites is the effect of incomplete filling on the strongly correlated electron phenomena and the R ion motions in the cage.We have carried out 121 Sb nuclear quadrupole resonance (NQR) and 139 La nuclear magnetic resonance (NMR) measurements by using almost completely filled materials of the heavy fermion YbFe 4 Sb 12 and the related compound LaFe 4 Sb 12 prepared at high pressures and high temperatures.2 The results of present NQR/NMR study are compared with the data previously reported for the compounds with rare-earth deficiencies of about 10%. Figure 1 shows 139 La (I = 7/2) NMR lines and 121 Sb (spin I = 5/2) NQR lines of the transition between | ± 3/2 and | ± 5/2 spin levels. Each of the Lorentzian-type resonance lines in shape has a *