Thermally activated exchange narrowing of the Gd3+ ESR fine structure in a single crystal of Ce1-xGdxFe4P12 (x = 0.001) skutterudite

We report electron spin resonance (ESR) measurements in the Gd3+ doped semiconducting filled skutterudite compound Ce1-xGdxFe4P12 (x = 0.001). As the temperature T varies from T = 150 K to T = 165 K, the Gd3+ ESR fine and hyperfine structures coalesce into a broad inhomogeneous single resonance. At T = 200 K the line narrows and as T increases further, the resonance becomes homogeneous with a thermal broadening of 1.1(2) Oe/K. These results suggest that the origin of these features may be associated to a subtle interdependence of thermally activated mechanisms that combine: i) an increase with T of the density of activated conduction-carriers across the T-dependent semiconducting pseudogap; ii) the Gd3+ Korringa relaxation process due to an exchange interaction, J_{fd}S.s, between the Gd3+ localized magnetic moments and the thermally activated conduction-carriers and; iii) a relatively weak confining potential of the rare-earth ions inside the oversized (Fe2P3)4 cage, which allows the rare-earths to become rattler Einstein oscillators above T = 148 K. We argue that the rattling of the Gd3+ ions, via a motional narrowing mechanism, also contributes to the coalescence of the ESR fine and hyperfine structure.Comment: 7 pages, 9 figures, accepted for publication in Phys Rev

Collapse of the Gd3+Gd^{3+} ESR fine structure throughout the coherent temperature of the Gd-doped Kondo Semiconductor CeFe4P12CeFe_{4}P_{12}

Experiments on the $Gd^{3+}$ Electron Spin Resonance (ESR) in the filled skutterudite $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$ ($x \approx 0.001$), 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 $T \approx K$), $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$ behaves as a Kondo-insulator with a relatively large hybridization gap, and the $Gd^{3+}$ 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 $T^{*} \approx 160 K$ 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 $Gd^{3+}$ 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 ($4.2$ - $300$ 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 $Gd^{3+}$ ESR fine structure observed in $Ce_{1-x}Gd_{x}Fe_{4}P_{12}$.Comment: 19 pages, 6 figure

Optimality and Complexity in Measured Quantum-State Stochastic Processes

If an experimentalist observes a sequence of emitted quantum states via either projective or positive-operator-valued measurements, the outcomes form a time series. Individual time series are realizations of a stochastic process over the measurements' classical outcomes. We recently showed that, in general, the resulting stochastic process is highly complex in two specific senses: (i) it is inherently unpredictable to varying degrees that depend on measurement choice and (ii) optimal prediction requires using an infinite number of temporal features. Here, we identify the mechanism underlying this complicatedness as generator nonunifilarity -- the degeneracy between sequences of generator states and sequences of measurement outcomes. This makes it possible to quantitatively explore the influence that measurement choice has on a quantum process' degrees of randomness and structural complexity using recently introduced methods from ergodic theory. Progress in this, though, requires quantitative measures of structure and memory in observed time series. And, success requires accurate and efficient estimation algorithms that overcome the requirement to explicitly represent an infinite set of predictive features. We provide these metrics and associated algorithms, using them to design informationally-optimal measurements of open quantum dynamical systems.Comment: 31 pages, 6 appendices, 22 figures; http://csc.ucdavis.edu/~cmg/compmech/pubs/qdic.ht

Nonlinear dynamics of coupled transverse-rotational waves in granular chains

The nonlinear dynamics of coupled waves in one-dimensional granular chains with and without a substrate is theoretically studied accounting for quadratic nonlinearity. The multiple time scale method is used to derive the nonlinear dispersion relations for infinite granular chains and to obtain the wave solutions for semiinfinite systems. It is shown that the sum-frequency and difference-frequency components of the coupled transverse-rotational waves are generated due to their nonlinear interactions with the longitudinal wave. Nonlinear resonances are not present in the chain with no substrate where these frequency components have low amplitudes and exhibit beating oscillations. In the chain positioned on a substrate two types of nonlinear resonances are predicted. At resonance, the fundamental frequency wave amplitudes decrease and the generated frequency component amplitudes increase along the chain, accompanied by the oscillations due to the wave numbers asynchronism. The results confirm the possibility of a highly efficient energy transfer between the waves of different frequencies, which could find applications in the design of acoustic devices for energy transfer and energy rectification