S. Paschen

Hall-effect evolution across a heavy-fermion quantum critical point

A quantum critical point (QCP) develops in a material at absolute zero when a new form of order smoothly emerges in its ground state. QCPs are of great current interest because of their singular ability to influence the finite temperature properties of materials. Recently, heavy-fermion metals have played a key role in the study of antiferromagnetic QCPs. To accommodate the heavy electrons, the Fermi surface of the heavy-fermion paramagnet is larger than that of an antiferromagnet. An important unsolved question is whether the Fermi surface transformation at the QCP develops gradually, as expected if the magnetism is of spin-density-wave (SDW) type, or suddenly, as expected if the heavy electrons are abruptly localized by magnetism. Here we report measurements of the low-temperature Hall coefficient (RH)—a measure of the Fermi surface volume—in the heavy-fermion metal YbRh2Si2 upon field-tuning it from an antiferromagnetic to a paramagnetic state. RH undergoes an increasingly rapid change near the QCP as the temperature is lowered, extrapolating to a sudden jump in the zero temperature limit. We interpret these results in terms of a collapse of the large Fermi surface and of the heavy-fermion state itself precisely at the QCP.

Atomic ordering and thermoelectric properties of the n-type clathrate Ba8Ni3.5Ge42.1□0.4

Single crystals of the type-I clathrate Ba(8)Ni(3.5)Ge(42.1)square(0.4) (space group Pm3n, no. 223, a = 10.798(2) A, l = 30 mm, slashed circle = 8 mm) were grown from the melt using the Bridgman technique. Their composition, determined by microprobe analysis, reveals a distinctly lower Ni content than previously reported for the lower limit (x = 5.4) of the homogeneity range of the clathrate-I phase Ba(8)Ni(x)Ge(46-x). From single crystal X-ray diffraction data we introduce a crystal structure model that takes point defects (vacancies) square in the Ge network into account. It reveals that both Ni and square accumulate at a single site (6c) and that, as a consequence, the Ge network distorts considerably. Ba(8)Ni(3.5)Ge(42.1)square(0.4) shows metal-like behaviour (drho/dT > 0) albeit with high resistivity at room temperature (rho(300 K) approximately 1 mOmega cm). Together with the low charge carrier concentration of 2.3 e(-)/unit cell at 300 K this is typical of a degenerate semiconductor. The lattice thermal conductivity is distinctly smaller than that of Ba(8)Ge(43)square(3), where the vacancies partially order, and smaller than those of Ba-Ni-Ge type-I clathrates without vacancies, suggesting that disordered vacancies efficiently scatter heat-transporting phonons. We provide evidence that the maximum value of the thermoelectric figure of merit reached in Ba(8)Ni(3.5)Ge(42.1)square(0.4), ZT(680 K) congruent with 0.21, can be further improved by adjusting the charge carrier concentration.

Fermi-surface collapse and dynamical scaling near a quantum-critical point

Quantum criticality arises when a macroscopic phase of matter undergoes a continuous transformation at zero temperature. While the collective fluctuations at quantum-critical points are being increasingly recognized as playing an important role in a wide range of quantum materials, the nature of the underlying quantum-critical excitations remains poorly understood. Here we report in-depth measurements of the Hall effect in the heavy-fermion metal YbRh2Si2, a prototypical system for quantum criticality. We isolate a rapid crossover of the isothermal Hall coefficient clearly connected to the quantum-critical point from a smooth background contribution; the latter exists away from the quantum-critical point and is detectable through our studies only over a wide range of magnetic field. Importantly, the width of the critical crossover is proportional to temperature, which violates the predictions of conventional theory and is instead consistent with an energy over temperature, E/T, scaling of the quantum-critical single-electron fluctuation spectrum. Our results provide evidence that the quantum-dynamical scaling and a critical Kondo breakdown simultaneously operate in the same material. Correspondingly, we infer that macroscopic scale-invariant fluctuations emerge from the microscopic many-body excitations associated with a collapsing Fermi-surface. This insight is expected to be relevant to the unconventional finite-temperature behavior in a broad range of strongly correlated quantum systems.

Destruction of the Kondo effect in the cubic heavy-fermion compound Ce3Pd20Si6

How ground states of quantum matter transform between one another reveals deep insights into the mechanisms stabilizing them. Correspondingly, quantum phase transitions are explored in numerous materials classes, with heavy-fermion compounds being among the most prominent ones. Recent studies in an anisotropic heavy-fermion compound have shown that different types of transitions are induced by variations of chemical or external pressure, raising the question of the extent to which heavy-fermion quantum criticality is universal. To make progress, it is essential to broaden both the materials basis and the microscopic parameter variety. Here, we identify a cubic heavy-fermion material as exhibiting a field-induced quantum phase transition, and show how the material can be used to explore one extreme of the dimensionality axis. The transition between two different ordered phases is accompanied by an abrupt change of Fermi surface, reminiscent of what happens across the field-induced antiferromagnetic to paramagnetic transition in the anisotropic YbRh2Si2. This finding leads to a materials-based global phase diagram--a precondition for a unified theoretical description.

Phononic filter effect of rattling phonons in the thermoelectric clathrate Ba8Ge40+xNi6-x.

One of the key requirements for good thermoelectric materials is a low lattice thermal conductivity. Here we present a combined neutron scattering and theoretical investigation of the lattice dynamics in the type I clathrate system Ba-Ge-Ni, which fulfills this requirement. We observe a strong hybridization between phonons of the Ba guest atoms and acoustic phonons of the Ge-Ni host structure over a wide region of the Brillouin zone, which is in contrast with the frequently adopted picture of isolated Ba atoms in Ge-Ni host cages. It occurs without a strong decrease of the acoustic phonon lifetime, which contradicts the usual assumption of strong anharmonic phonon-phonon scattering processes. Within the framework of ab initio density-functional theory calculations we interpret these hybridizations as a series of anticrossings which act as a low-pass filter, preventing the propagation of acoustic phonons. To highlight the effect of such a phononic low-pass filter on the thermal transport, we compute the contribution of acoustic phonons to the thermal conductivity of Ba8Ge40Ni6 and compare it to those of pure Ge and a Ge-46 empty-cage model system.

Are type-I clathrates Zintl phases and 'phonon glasses and electron single crystals'?

Abstract We discuss to which extent the concepts of Zintl phases and of ‘phonon glasses and electron single crystals’ apply to type-I clathrates. In (β-) Eu 8 Ga 16 Ge 30 the presence of residual charge carriers appears to be related to a slight off-stoichiometry of the samples pointing to the validity of the Zintl concept in stoichiometric samples. The low and almost stoichiometry independent mobilities of (β-) Eu 8 Ga 16 Ge 30 , Sr 8 Ga 16 Ge 30 , and Ba 8 Ga 16 Ge 30 seriously question the validity of the ‘electron single crystal’ concept for type-I clathrates. The temperature dependence of the thermal conductivity of a Ba 8 Ga 16 Ge 30 single crystal indicates that tunneling states play a central role in producing ‘phonon glass’-like thermal conductivities.

Evidence for a non-Fermi-liquid phase in Ge-substituted YbRh2Si2.

The canonical view of heavy fermion quantum criticality assumes a single quantum critical point separating the paramagnet from the antiferromagnet. However, recent experiments on Yb-based heavy fermion compounds suggest the presence of non-Fermi liquid behavior over a finite zero-temperature region. Using detailed susceptibility and transport measurements we show that the classic quantum critical system, Ge-substituted YbRh(2)Si(2), also displays such behavior. We advance arguments that this is not due to a disorder-smeared quantum critical point, but represents a new class of metallic phase.

Introducing a Magnetic Guest to a Tetrel-Free Clathrate: Synthesis, Structure, and Properties of EuxBa8–xCu16P30 (0 ≤ x ≤ 1.5)

The europium-containing clathrate-I Eu(x)Ba(8-x)Cu(16)P(30) was synthesized from the elements. Powder X-ray diffraction in combination with energy dispersive X-ray absorption spectroscopy (EDXS) and metallographic studies showed the homogeneity range with x ≤ 1.5. Determination of the crystal structure confirmed the presence of an orthorhombic superstructure of clathrate-I and revealed that Eu atoms exclusively resided in small pentagonal-dodecahedral cages. Magnetic measurements together with X-ray absorption spectroscopy are consistent with a 4f(7) (Eu(2+)) ground state for Eu(x)Ba(8-x)Cu(16)P(30). Below 3 K the Eu moments order antiferromagnetically. Resistivity measurements revealed metallic behavior of the investigated clathrate, in line with the composition deviating from the Zintl counting scheme. Local vibrations of the guest atoms inside the cages are analyzed with the help of specific heat investigations.

Thermoelectric properties of Ba-Cu-Si clathrates

(Dated: November 15, 2011) Thermoelectric properties of the type-I clathrates Ba8CuxSi46−x (3.6 � x � 7, x = nominal Cu content) are investigated both experimentally and theoretically. The polycrystalline samples are prepared either by melting, ball milling and hot pressing or by melt spinning, hand milling and hot pressing techniques. Temperature-dependent electrical resistivity, �(T), and the Seebeck coefficient, S(T), measurements reveal metal-like behavior for all samples. For x = 5 and 6, density functional theory calculations are performed for deriving the enthalpy of formation and the electronic structure which is exploited for the calculation of Seebeck coefficients and conductivity within Boltzmann’s transport theory. For simulating the properties of doped clathrates the rigid band model is applied. On the basis of the density functional theory results the experimentally observed compositional dependence of �(T) and S(T) of the whole sample series is analyzed. The highest dimensionless thermoelectric figure of merit ZT of 0.28 is reached for a melt-spun sample at 600 ◦ C. The relatively low ZT values in this system are attributed to the too high charge carrier concentrations.

Quantum phase transitions in heavy fermion metals and Kondo insulators

Strongly correlated electron systems at the border of magnetism are of active current interest, particularly because the accompanying quantum criticality provides a route towards both strange-metal non-Fermi liquid behavior and unconventional superconductivity. Among the many important questions is whether the magnetism acts simply as a source of fluctuations in the textbook Landau framework, or instead serves as a proxy for some unexpected new physics. We put into this general context the recent developments on quantum phase transitions in antiferromagnetic heavy fermion metals. Among these are the extensive recent theoretical and experimental studies on the physics of Kondo destruction in a class of beyond-Landau quantum critical points. Also discussed are the theoretical basis for a global phase diagram of antiferromagnetic heavy fermion metals, and the recent surge of materials suitable for studying this phase diagram. Furthermore, we address the generalization of this global phase diagram to the case of Kondo insulators, and consider the future prospect to study the interplay among Kondo coherence, magnetism and topological states. Finally, we touch upon related issues beyond the antiferromagnetic settings, arising in mixed valent, ferromagnetic, quadrupolar, or spin glass f-electron systems, as well as some general issues on emergent phases near quantum critical points.