13,066 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
Collapse of the ESR fine structure throughout the coherent temperature of the Gd-doped Kondo Semiconductor
Experiments on the Electron Spin Resonance (ESR) in the filled
skutterudite (), at temperatures
where the host resistivity manifests a smooth insulator-metal crossover,
provides evidence of the underlying Kondo physics associated with this system.
At low temperatures (below ), behaves
as a Kondo-insulator with a relatively large hybridization gap, and the
ESR spectra displays a fine structure with lorentzian line shape,
typical of insulating media. The electronic gap is attributed to the large
hybridization present in the coherent regime of a Kondo lattice, when Ce
4f-electrons cooperate with band properties at half-filling. Mean-field
calculations suggest that the electron-phonon interaction is fundamental at
explaining the strong 4f-electron hybridization in this filled skutterudite.
The resulting electronic structure is strongly temperature dependent, and at
about the system undergoes an insulator-to-metal
transition induced by the withdrawal of 4f-electrons from the Fermi volume, the
system becoming metallic and non-magnetic. The ESR fine structure
coalesces into a single dysonian resonance, as in metals. Still, our
simulations suggest that exchange-narrowing via the usual Korringa mechanism,
alone, is not capable of describing the thermal behavior of the ESR spectra in
the entire temperature region ( - K). We propose that temperature
activated fluctuating-valence of the Ce ions is the missing ingredient that,
added to the usual exchange-narrowing mechanism, fully describes this unique
temperature dependence of the ESR fine structure observed in
.Comment: 19 pages, 6 figure
Anomalous infrared spectra of hybridized phonons in type-I clathrate BaGaGe
The optical conductivity spectra of the rattling phonons in the clathrate
BaGaGe are investigated in detail by use of the terahertz
time-domain spectroscopy. The experiment has revealed that the lowest-lying
vibrational mode of a Ba(2) ion consists of a sharp Lorentzian peak at
1.2 THz superimposed on a broad tail weighted in the lower frequency regime
around 1.0 THz. With decreasing temperature, an unexpected linewidth broadening
of the phonon peak is observed, together with monotonic softening of the phonon
peak and the enhancement of the tail structure. These observed anomalies are
discussed in terms of impurity scattering effects on the hybridized phonon
system of rattling and acoustic phonons.Comment: Submitted to JPS
Eu2+ spin dynamics in the filled skutterudites EuM4Sb12 (M = Fe, Ru, Os)
We report evidence for a close relation between the thermal activation of the
rattling motion of the filler guest atoms, and inhomogeneous spin dynamics of
the Eu2+ spins. The spin dynamics is probed directly by means of Eu2+ electron
spin resonance (ESR), performed in both X-band (9.4 GHz) and Q-band (34 GHz)
frequencies in the temperature interval 4.2 < T < 300 K. A comparative study
with ESR measurements on the Beta-Eu8Ga16Ge30 clathrate compound is presented.
Our results point to a correlation between the rattling motion and the spin
dynamics which may be relevant for the general understanding of the dynamics of
cage systems.Comment: 6 pages, 4 figures, accepted for publication in Phys. Rev.
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