3 research outputs found
Cage-size control of guest vibration and thermal conductivity in Sr8Ga16Si30-xGex
We present a systematic study of thermal conductivity, specific heat,
electrical resistivity, thermopower and x-ray diffraction measurements
performed on single-crystalline samples of the pseudoquaternary type-I
clathrate system Sr8Ga16Si30-xGex, in the full range of 0 < x < 30. All the
samples show metallic behavior with n-type majority carriers. However, the
thermal conductivity and specific heat strongly depend on x. Upon increasing x
from 0 to 30, the lattice parameter increases by 3%, from 10.446 to 10.726 A,
and the localized vibrational energies of the Sr guest ions in the
tetrakaidekahedron (dodecahedron) cages decrease from 59 (120) K to 35 (90) K.
Furthermore, the lattice thermal conductivity at low temperatures is largely
suppressed. In fact, a crystalline peak found at 15 K for x = 0 gradually
decreases and disappears for x > 20, evolving into the anomalous glass-like
behavior observed for x = 30. It is found that the increase of the free space
for the Sr guest motion directly correlates with a continuous transition from
on-center harmonic vibration to off-center anharmonic vibration, with
consequent increase in the coupling strength between the guest's low-energy
modes and the cage's acoustic phonon modes.Comment: 7 pages, 7 figures, submitted to PR