Showing papers by "Silke Paschen published in 2019"

Kondo-like phonon scattering in thermoelectric clathrates.

Abstract: Crystalline solids are generally known as excellent heat conductors, amorphous materials or glasses as thermal insulators. It has thus come as a surprise that certain crystal structures defy this paradigm. A prominent example are type-I clathrates and other materials with guest-host structures. They sustain low-energy Einstein-like modes in their phonon spectra, but are also prone to various types of disorder and phonon-electron scattering and thus the mechanism responsible for their ultralow thermal conductivities has remained elusive. Our thermodynamic and transport measurements on various clathrate single crystal series and their comparison with ab initio simulations reveal an all phononic Kondo effect as origin. This insight devises design strategies to further suppress the thermal conductivity of clathrates and other related materials classes, with relevance for thermoelectric waste heat recovery and, more generally, phononic applications. It may also trigger theoretical work on strong correlation effects in phonon systems.

Highly anisotropic interlayer magnetoresitance in ZrSiS nodal-line Dirac semimetal

Abstract: We instigate the angle-dependent magnetoresistance (AMR) of the layered nodal-line Dirac semimetal ZrSiS for the in-plane and out-of-plane current dir

Sequential localization of a complex electron fluid.

Abstract: Complex and correlated quantum systems with promise for new functionality often involve entwined electronic degrees of freedom. In such materials, highly unusual properties emerge and could be the result of electron localization. Here, a cubic heavy fermion metal governed by spins and orbitals is chosen as a model system for this physics. Its properties are found to originate from surprisingly simple low-energy behavior, with 2 distinct localization transitions driven by a single degree of freedom at a time. This result is unexpected, but we are able to understand it by advancing the notion of sequential destruction of an SU(4) spin–orbital-coupled Kondo entanglement. Our results implicate electron localization as a unified framework for strongly correlated materials and suggest ways to exploit multiple degrees of freedom for quantum engineering.

Low-carrier density and fragile magnetism in a Kondo lattice system

Abstract: Kondo-based semimetals and semiconductors are of extensive current interest as a viable platform for strongly correlated states. It is thus important to understand the routes towards such dilute-carrier correlated states. One established pathway is through Kondo effect in metallic non-magnetic analogues. Here we advance a new mechanism, through which Kondo-based semimetals develop out of conduction electrons with a low carrier-density in the presence of an even number of rare-earth sites. We demonstrate this effect by studying the Kondo material Yb3Ir4Ge13 along with its closed-f-shell counterpart, Lu3Ir4Ge13. Through magnetotransport, optical conductivity and thermodynamic measurements, we establish that the correlated semimetallic state of Yb3Ir4Ge13 below its Kondo temperature originates from the Kondo effect of a low carrier conduction-electron background. In addition, it displays fragile magnetism at very low temperatures, which, in turn, can be tuned to a non Fermi liquid regime through Lu-for-Yb substitution. These findings are connected with recent theoretical studies in simplified models. Our results open an entirely new venue to explore the strong correlation physics in a semimetallic environment.

Robust scheme for magnetotransport analysis in topological insulators

Abstract: The recent excitement about Dirac and Weyl fermion systems has renewed interest in magnetotransport properties of multicarrier systems. However, the complexity of their analysis, even in the simplest two-carrier case, has hampered a good understanding of the underlying phenomena. Here we propose a new analysis scheme for two independent conduction channels, that strongly reduces previous ambiguities and allows one to draw robust conclusions. This is demonstrated explicitly for the example of three-dimensional topological insulators. Their temperature and gate voltage-dependent Hall coefficient and transverse magnetoresistance behavior, including the phenomenon of huge linear transverse magnetoresistance, can be traced back to two conduction channels, with fully determined carrier concentrations and mobilities. We further derive an upper limit for the transverse magnetoresistance. Its violation implies field dependencies in the electronic band structure or scattering processes, or the presence of more than two effective carrier types. Remarkably, none of the three-dimensional topological insulators or semimetals with particularly large transverse magnetoresistance violates this limit.

Dynamical Kondo effect and Kondo destruction in effective models for quantum-critical heavy fermion metals

Abstract: Quantum criticality in certain heavy-fermion metals is believed to go beyond the Landau framework of order-parameter fluctuations. In particular, there is considerable evidence for Kondo destruction: a disappearance of the static Kondo singlet amplitude that results in a sudden reconstruction of Fermi surface across the quantum critical point and an extra critical energy scale. This effect can be analyzed in terms of a dynamical interplay between the Kondo and RKKY interactions. In the Kondo-destroyed phase, a well-defined Kondo resonance is lost, but Kondo singlet correlations remain at nonzero frequencies. This dynamical effect allows for mass enhancement in the Kondo-destroyed phase. Here, we elucidate the dynamical Kondo effect in Bose-Fermi Kondo/Anderson models, which unambiguously exhibit Kondo-destruction quantum critical points. We show that a simple physical quantity---the expectation value $\langle {\bf S}_{f} \cdot {\bf s}_{c} \rangle$ for the dot product of the local ($f$) and conduction-electron ($c$) spins---varies continuously across such quantum critical points. A nonzero $\langle {\bf S}_{f} \cdot {\bf s}_{c} \rangle$ manifests the dynamical Kondo effect that operates in the Kondo-destroyed phase. Implications are discussed for the stability of Kondo-destruction quantum criticality as well as the understanding of experimental results in quantum critical heavy-fermion metals.

Evolution of the propagation vector of antiferroquadrupolar phases in Ce 3 Pd 20 Si 6 under magnetic field

Abstract: Hidden-order phases that occur in a number of correlated $f$-electron systems are among the most elusive states of electronic matter. Their investigations are hindered by the insensitivity of standard physical probes, such as neutron diffraction, to the order parameter that is usually associated with higher-order multipoles of the $f$ orbitals. The heavy-fermion compound ${\mathrm{Ce}}_{3}{\mathrm{Pd}}_{20}{\mathrm{Si}}_{6}$ exhibits magnetically hidden order at subkelvin temperatures, known as phase II. Additionally, for magnetic field applied along the [001] cubic axis, another phase ${\mathrm{II}}^{\ensuremath{'}}$ was detected, but the nature of the transition from phase II to phase ${\mathrm{II}}^{\ensuremath{'}}$ remained unclear. Here we use inelastic neutron scattering to argue that this transition is most likely associated with a change in the propagation vector of the antiferroquadrupolar order from (111) to (100). Despite the absence of magnetic Bragg scattering in phase ${\mathrm{II}}^{\ensuremath{'}}$, its ordering vector is revealed by the location of an intense magnetic soft mode at the (100) wave vector, that is orthogonal to the applied field. At the II-${\mathrm{II}}^{\ensuremath{'}}$ transition, this mode softens and transforms into quasielastic and nearly $\mathbf{Q}$-independent incoherent scattering, which is likely related to the non-Fermi-liquid behavior recently observed at this transition. Our experiment also reveals sharp collective excitations in the field-polarized paramagnetic phase, after phase ${\mathrm{II}}^{\ensuremath{'}}$ is suppressed in fields above 4 T.

Structural and Thermoelectric Properties of Cu Substituted Type I Clathrates Ba8CuxSi~32−xGa~14

Abstract: With an attempt to improve the thermoelectric properties of type I clathrates in the Ba-Ga-Si system, we introduce Cu into the framework of the crystal structure. Single crystals are prepared in Ga-flux and characterized by X-ray diffraction techniques and transport measurements for the structural and thermoelectric properties. Our composition analyses show that only a small amount of Cu is determined in the clathrates. The single crystal X-ray diffraction data refinements confirm that Ga atoms prefer the 6c and 24k sites and avoid the 16i sites in the crystal structure. The small amount of Cu affects the crystal structure by compressing the tetrakaidecahedral cage along the direction perpendicular to the six-atom-ring plane. This could be the reason for the high charge carrier concentration, and low electrical resistivity and Seebeck coefficient. We analyze the principal mechanism for our observation and conclude that the Cu substitution can adjust some subtle details of the structure, maintaining the Zintl rule in the type I clathrates.

Quenching a Weyl-Kondo semimetal by magnetic field

Abstract: With the advent of topology in electronic materials the number of predicted quantum phases has literally exploded. Most of them, however, still await firm experimental identification. In strongly correlated electron systems, scanning their low-temperature phase diagrams by varying a nonthermal control parameter has been instrumental in delineating phases defined by a Landau order parameter. Here we show that this approach is versatile also for strongly correlated topological phases. We use Hall effect measurements to probe how the time reversal symmetry invariant Weyl-Kondo semimetal Ce$_3$Bi$_4$Pd$_3$ transforms under magnetic-field tuning. We detect an intriguing two-stage transition, which we associate with an annihilation of the Weyl nodes, making the system more insulating, and a consecutive transition to a heavy fermion metal phase. We expect our work to stimulate tuning studies in related systems, thereby advancing the much needed identification of organizing principles for strongly correlated electronic topology.

Thermal conductivity of the Kondo semiconductor CeRu$_4$Sn$_6$

Abstract: We report measurements of the thermal conductivity $\kappa$ on single crystalline CeRu$_4$Sn$_6$ in the temperature range between 80mK and 80K, along the main crystallographic directions. $\kappa$ is phonon-dominated in the whole temperature range and is found to be essentially isotropic. At low temperatures the data are well approximated by $\kappa \propto T^2$, which is attributed to a predominant scattering of phonons on electrons. We describe the data with a Callaway fit in the whole temperature range giving good agreement at low and high temperatures.

Controlling electronic topology in a strongly correlated electron system.

Abstract: Combining strong electron correlations [1-4] and nontrivial electronic topology [5] holds great promise for discovery. So far, this regime has been rarely accessed and systematic studies are much needed to advance the field. Here we demonstrate the control of topology in a heavy fermion system. We use magnetic field to manipulate Weyl nodes in a Weyl-Kondo semimetal [6-8], up to the point where they annihilate in a topological quantum phase transition. The suppression of the topological characteristics occurs in an intact and only weakly varying strongly correlated "background". Thus, topology is changing per se and not as a consequence of a change of the correlation state, for instance across a magnetic, electronic or structural phase transition. Our demonstration of genuine topology tuning in a strongly correlated electron system sets the stage for establishing global phase diagrams of topology, an approach that has proven highly valuable to explore and understand topologically trivial strongly correlated electron systems [1-4]. Our work also lays the ground for technological exploitations of controlled electronic topology.

$^{105}$Pd NMR and NQR study of the cubic heavy fermion system Ce$_3$Pd$_{20}$Si$_6$

Abstract: We report $^{105}$Pd NMR and NQR measurements on a single crystal of Ce$_3$Pd$_{20}$Si$_6$, where antiferroquadrupolar and antiferromagnetic orders develop at low temperature. From the analysis of NQR and NMR spectra, we have determined the electric field gradient (EFG) tensors and the anisotropic Knight shift ($K$) components for both inequivalent Pd sites - Pd($32f$) and Pd($48h$). The observed EFG values are in excellent agreement with our state-of-the-art DFT calculations. The principal values of the quadrupolar coupling are $(20.37 \pm 0.02)$ MHz and $(5.45 \pm 0.02)$ MHz, for the Pd($32f$) and Pd($48h$) site, respectively, which is large compared to the Larmor frequency defined by the gyromagnetic constant $\gamma = 1.94838$ MHz/T for $^{105}$Pd. Therefore, the complete knowledge of $K$ and the EFG tensors is crucial to establish the correspondence between NMR spectra and crystallographic sites, which is needed for a complete analysis of the magnetic structure, static spin susceptibility, and the spin-lattice relaxation rate data and a better understanding of the groundstate of Ce$_3$Pd$_{20}$Si$_6$.

Strange metal near antiferromagnetic instability and Kondo breakdown in heavy-fermion systems

Abstract: The strange metal behavior with T-linear resistivity and T-logarithmic specific heat coefficient has been widely observed in heavy-fermion metals close to antiferromagnetic transitions. The underlying mechanism leading to this behavior constitutes an outstanding and largely unresolved issue. An increasing amount of experiments indicates a link to a Kondo breakdown quantum critical point. To investigate this, we study the 2D Kondo-Heisenberg model via a dynamical large-N multichannel Schwinger boson approach. We identify and characterize the quantum critical point separating the antiferromagnetically ordered from the Kondo-screened heavy Fermi-liquid phases. In addition, we find strange-metal behavior in the finite temperature phase diagram close to the transition which agrees qualitatively with the experimental results on CeCu_{6-x}Au_{x}, YbRh_{2}Si_{2}, and others.