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S. Paschen

Publications and source records attributed to S. Paschen.

At least 19 recordsLinked to original sources

Dynamical magnetotropic susceptibility as a new probe of Kitaev materials and beyond

The magnetotropic susceptibility $k(\omega)$ probes ultra-low-frequency uniform fluctuations. For a crystal mounted on an oscillating cantilever in a magnetic field, it is defined as the ratio of torque to angular-displacement amplitude. Its real and imaginary parts determine the oscillation-frequency shift and crystal-induced damping. It is a low-energy probe of uniform $q=0$ spin and charge degrees of freedom. We demonstrate this by deriving $k(\omega)$ within linear response theory for a generic correlated-electron Hamiltonian with charge and spin degrees of freedom. Although it covers metallic and insulating magnets, correlated paramagnets, and exotic quantum critical points, we focus on limiting cases. For insulating spin systems $k(0)$ is sensitive to magnetic anisotropy whereas its finite-frequency imaginary part probes uniform dynamical spin susceptibility even in spin-symmetric models. For metallic systems we identify when eddy currents cause low-frequency damping. Our numerical results focus on Kitaev-material magnetotropic response. Using auxiliary-field quantum Monte Carlo with machine-learning-based sign-problem optimization we compute $k(\omega)$ for several models proposed for $\alpha$-RuCl$_3$. The observed low-temperature scaling of $k(0)/T$ with $B/T$ results from dominant Kitaev couplings: parameter sets without dominant Kitaev coupling do not exhibit this scaling. It remains robust upon inclusion of optical phonons. Beyond the static response, $k''(\omega)$ for the $\alpha$-RuCl$_3$ parameter set reproducing the experimental $k(0)$ data shows local-moment features at high and low $T$, with a single peak at the Larmor frequency. Beyond Kitaev systems we highlight broader applications. Probing ultra-low-energy uniform charge fluctuations is pertinent to Kondo destruction quantum criticality, of broad interest in strange metallicity and unconventional superconductivity.

cond-mat.str-el

Emergent Topological Semimetal

A material's electronic topology, which is generally described via its Bloch states and the associated bandstructure, will be enriched by the presence of interactions. In metallic settings, the interactions are usually treated through the concept of quasiparticles. Using the genuinely quantum critical heavy fermion compound CeRu$_4$Sn$_6$, we investigate what happens if no well-defined quasiparticles are present. Surprisingly, we discover a topological semimetal phase that emerges from the material's quantum critical state and exhibits a dome structure as a function of magnetic field and pressure. To understand these results, we study a Weyl-Kondo semimetal model at a Kondo destruction quantum critical point. Indeed, it exhibits features in the spectral function that can define topological crossings beyond the quasiparticle picture. We expect our work to stimulate the search for other emergent topological phases.

cond-mat.str-el

Ce$_3$Bi$_4$Ni$_3$ $-$ A large hybridization-gap variant of Ce$_3$Bi$_4$Pt$_3$

The family of cubic noncentrosymmetric 3-4-3 compounds has become a fertile ground for the discovery of novel correlated metallic and insulating phases. Here, we report the synthesis of a new heavy fermion compound, Ce$_3$Bi$_4$Ni$_3$. It is an isoelectronic analog of the prototypical Kondo insulator Ce$_3$Bi$_4$Pt$_3$ and of the recently discovered Weyl-Kondo semimetal Ce$_3$Bi$_4$Pd$_3$. In contrast to the volume-preserving Pt-Pd substitution, structural and chemical analyses reveal a positive chemical pressure effect in Ce$_3$Bi$_4$Ni$_3$ relative to its heavier counterparts. Based on the results of electrical resistivity, Hall effect, magnetic susceptibility, and specific heat measurements, we identify an energy gap of 65-70 meV, about eight times larger than that in Ce$_3$Bi$_4$Pt$_3$ and about 45 times larger than that of the Kondo-insulating background hosting the Weyl nodes in Ce$_3$Bi$_4$Pd$_3$. We show that this gap as well as other physical properties do not evolve monotonically with increasing atomic number, i.e., in the sequence Ce$_3$Bi$_4$Ni$_3$-Ce$_3$Bi$_4$Pd$_3$-Ce$_3$Bi$_4$Pt$_3$, but instead with increasing partial electronic density of states of the $d$ orbitals at the Fermi energy. To understand under which condition topological states form in these materials is a topic for future studies.

cond-mat.str-el

Anomalous Shubnikov-de Haas effect and observation of the Bloch-Gr\"uneisen temperature in the Dirac semimetal ZrTe5

Appearance of quantum oscillations (QO) in both thermodynamic and transport properties of metals at low temperatures is the most striking experimental consequence of the existence of a Fermi surface (FS). The frequency of these oscillations and the temperature dependence of their amplitude provides essential information about the FS topology and fermionic quasiparticle properties. Here, we report the observation of an anomalous suppression of the QO amplitude seen in resistivity (Shubnikov de-Haas effect) at sub-kelvin temperatures in ZrTe5 samples with a single small FS sheet comprising less than 5% of the first Brillouin zone. By comparing these results with measurements of the magneto-acoustic QO and the recovery of the usual Lifshitz-Kosevich behavior of the Shubnikov de-Haas (SdH) effect in ZrTe$_5$ samples with a multi-sheet FS, we show that the suppression of the SdH effect originates from a decoupling of the electron liquid from the lattice. On crossing the so-called Bloch-Gr\"uneisen temperature, T$_BG$, electron-phonon scattering becomes strongly suppressed and in the absence of Umklapp scattering the electronic liquid regains Galilean invariance. In addition, we show, using a combination of zero-field electrical conductivity and ultrasonic-absorption measurements, that entering this regime leads to an abrupt increase of electronic viscosity.

cond-mat.mtrl-sci

Evidence of 3D Dirac conical bands in TlBiSSe by optical and magneto-optical spectroscopy

TlBiSSe is a rare realization of a 3D semimetal with a conically dispersing band that has an optical response which is well isolated from other contributions in a broad range of photon eneries. We report optical and magneto-optical spectroscopy on this material. When the compound is chemically tuned into a state of the lowest carrier concentration, we find a nearly linear frequency dependence of the optical conductivity below 0.5~eV. Landau level spectroscopy allows us to describe the system with a massive Dirac model, giving a gap $2\Delta =32$~meV and an in-plane velocity parameter $v= 4.0\times 10^5$~m/s. % Finally, we provide a theoretical recipe to extract all parameters of the anisotropic Dirac band, including the Fermi energy and band degeneracy.

cond-mat.mtrl-sci

Cascade of magnetic-field-driven quantum phase transitions in Ce3Pd20Si6

Magnetically hidden order is a hypernym for electronic ordering phenomena that are visible to macroscopic thermodynamic probes but whose microscopic symmetry cannot be revealed with conventional neutron or x-ray diffraction. In a handful of f-electron systems, the ordering of odd-rank multipoles leads to order parameters with a vanishing neutron cross-section. Among them, Ce$_3$Pd$_{20}$Si$_6$ is known for its unique phase diagram exhibiting two distinct multipolar-ordered ground states (phases II and II'), separated by a field-driven quantum phase transition associated with a putative change in the ordered quadrupolar moment from $O_2^0$ to $O_{xy}$. Using torque magnetometry at subkelvin temperatures, here we find another phase transition at higher fields above 12 T, which appears only for low-symmetry magnetic field directions $\mathbf{B} \parallel \langle11L\rangle$ with $1 < L \leq 2$. While the order parameter of this new phase II'' remains unknown, the discovery renders Ce$_3$Pd$_{20}$Si$_6$ a unique material with two field-driven phase transitions between distinct multipolar phases. They are both clearly manifested in the magnetic-field dependence of the field-induced (111) Bragg intensities measured with neutron scattering for $\mathbf{B} \parallel [112]$. We also find from inelastic neutron scattering that the number of nondegenerate collective excitations induced by the magnetic field correlates with the number of phases in the magnetic phase diagram for the same field direction. Furthermore, the magnetic excitation spectrum suggests that the new phase II'' may have a different propagation vector, revealed by the minimum in the dispersion that may represent the Goldstone mode of this hidden-order phase.

cond-mat.str-el

Superconductivity in an extreme strange metal

Some of the highest-transition-temperature superconductors across various materials classes exhibit linear-in-temperature `strange metal' or `Planckian' electrical resistivities in their normal state. It is thus believed by many that this behavior holds the key to unlock the secrets of high-temperature superconductivity. However, these materials typically display complex phase diagrams governed by various competing energy scales, making an unambiguous identification of the physics at play difficult. Here we use electrical resistivity measurements into the micro-Kelvin regime to discover superconductivity condensing out of an extreme strange metal state -- with linear resistivity over 3.5 orders of magnitude in temperature. We propose that the Cooper pairing is mediated by the modes associated with a recently evidenced dynamical charge localization-delocalization transition, a mechanism that may well be pertinent also in other strange metal superconductors.

cond-mat.supr-con

Pristine quantum criticality in a Kondo semimetal

The observation of quantum criticality in diverse classes of strongly correlated electron systems has been instrumental in establishing ordering principles, discovering new phases, and identifying the relevant degrees of freedom and interactions. At focus so far have been insulators and metals. Semimetals, which are of great current interest as candidate phases with nontrivial topology, are much less explored in experiments. Here we study the Kondo semimetal CeRu$_4$Sn$_6$ by magnetic susceptibility, specific heat, and inelastic neutron scattering experiments. The power-law divergence of the magnetic Grünesien ratio reveals that, surprisingly, this compound is quantum critical without tuning. The dynamical energy over temperature scaling in the neutron response, seen throughout the Brillouin zone, as well as the temperature dependence of the static uniform susceptibility indicate that temperature is the only energy scale in the criticality. Such behavior, which has been associated with Kondo destruction quantum criticality in metallic systems, may well be generic in the semimetal setting.

cond-mat.str-el

Switching on surface conduction in a topological insulator

The protected surface conduction of topological insulators is in high demand for the next generation of electronic devices. What is needed to move forward are robust settings where topological surface currents can be controlled by simple means, ideally by the application of external stimuli. Surprisingly, this direction is only little explored. In this work we demonstrate that we can boost the surface conduction of a topological insulator by both light and electric field. This happens in a fully controlled way, and the additional Dirac carriers exhibit ultra-long lifetimes. We provide a comprehensive understanding, namely that carriers are injected from the bulk to the surface states across an intrinsic Schottky barrier. We expect this mechanism to be at play in a broad range of materials and experimental settings.

cond-mat.mtrl-sci

Sequential localization of a complex electron fluid

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 two 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.

cond-mat.str-el

Nanostructured clathrates and clathrate-based nanocomposites

Intermetallic clathrates are candidate materials for thermoelectric applications above room temperature. Here we explore whether their intrinsically low lattice thermal conductivities can be further reduced by nanostructuring and whether this can further enhance their thermoelectric performance.}{As bulk nanostructuring routes we studied melt spinning and ball milling. To optimize the compaction process and/or stabilize the nanostructure we varied the process parameters, used additives, and studied clathrate-based composites. Initial results on clathate nanowires as simpler model nanostructures are also presented.

cond-mat.mtrl-sci

Evolution of the propagation vector of antiferroquadrupolar phases in Ce3Pd20Si6 with magnetic field

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 Ce3Pd20Si6 exhibits magnetically hidden order at subkelvin temperatures, known as phase II. Additionally, for magnetic field applied along the [001] cubic axis, another phase II' was detected, but the nature of the transition from phase II to phase II' remained unclear. Here we use inelastic neutron scattering to demonstrate that this transition is 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 II', its ordering vector is revealed by the location of an intense magnetic soft mode at the (100) wave vector, orthogonal to the applied field. At the II-II' transition, this mode softens and transforms into quasielastic and nearly 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 II' is suppressed in fields above 4 T.

cond-mat.str-el

Highly anisotropic interlayer magnetoresistance in ZrSiS nodal-line Dirac semimetal

We instigate the angle-dependent magnetoresistance (AMR) of the layered nodal-line Dirac semimetal ZrSiS for the in-plane and out-of-plane current directions. This material has recently revealed an intriguing butterfly-shaped in-plane AMR that is not well understood. Our measurements of the polar out-of-plane AMR show a surprisingly different response with a pronounced cusp-like feature. The maximum of the cusp-like anisotropy is reached when the magnetic field is oriented in the $a$-$b$ plane. Moreover, the AMR for the azimuthal out-of-plane current direction exhibits a very strong four-fold $a$-$b$ plane anisotropy. Combining the Fermi surfaces calculated from first principles with the Boltzmann's semiclassical transport theory we reproduce and explain all the prominent features of the unusual behavior of the in-plane and out-of-plane AMR. We are also able to clarify the origin of the strong non-saturating transverse magnetoresistance as an effect of imperfect charge-carrier compensation and open orbits. Finally, by combining our theoretical model and experimental data we estimate the average relaxation time of $2.6\times10^{-14}$~s and the mean free path of $15$~nm at 1.8~K in our samples of ZrSiS.

cond-mat.mtrl-sci

Robust scheme for magnetotransport analysis in topological insulators

The recent excitement about Dirac and Weyl fermion systems has renewed interest in magnetotransport properties of multi-carrier 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 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 dependences 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.

cond-mat.mes-hall

Singular charge fluctuations at a magnetic quantum critical point

Strange metal behavior is ubiquitous to correlated materials ranging from cuprate superconductors to bilayer graphene. There is increasing recognition that it arises from physics beyond the quantum fluctuations of a Landau order parameter which, in quantum critical heavy fermion antiferromagnets, may be realized as critical Kondo entanglement of spin and charge. The dynamics of the associated electronic delocalization transition could be ideally probed by optical conductivity, but experiments in the corresponding frequency and temperature ranges have remained elusive. We present terahertz time-domain transmission spectroscopy on molecular beam epitaxy-grown thin films of YbRh$_2$Si$_2$, a model strange metal compound. We observe frequency over temperature scaling of the optical conductivity as a hallmark of beyond-Landau quantum criticality. Our discovery implicates critical charge fluctuations as playing a central role in the strange metal behavior, thereby elucidating one of the longstanding mysteries of correlated quantum matter.

cond-mat.str-el

Kondo-like phonon scattering in thermoelectric clathrates

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. While recent ab initio lattice dynamics simulations show that the Einstein-like modes enhance phonon-phonon Umklapp scattering, they reproduce experimental data only at low temperatures. Here we show that a new effect, an "all phononic Kondo effect", can resolve this discrepancy. This is evidenced by our thermodynamic and transport measurements on various clathrate single crystal series and their comparison with ab initio simulations. Our new understanding devises design strategies to further suppress the thermal conductivity of clathrates and other related materials classes, with relevance for the field of thermoelectric waste heat recovery but also more generally for phononic applications. More fundamentally, it may trigger theoretical work on strong correlation effects in phonon systems.

cond-mat.str-el

Kondo Insulator to Semimetal Transformation Tuned by Spin-Orbit Coupling

Recent theoretical studies of topologically nontrivial electronic states in Kondo insulators have pointed to the importance of spin-orbit coupling (SOC) for stabilizing these states. However, systematic experimental studies that tune the SOC parameter $λ_{\rm{SOC}}$ in Kondo insulators remain elusive. The main reason is that variations of (chemical) pressure or doping strongly influence the Kondo coupling $J_{\text{K}}$ and the chemical potential $μ$ -- both essential parameters determining the ground state of the material -- and thus possible $λ_{\rm{SOC}}$ tuning effects have remained unnoticed. Here we present the successful growth of the substitution series Ce$_3$Bi$_4$(Pt$_{1-x}$Pd$_x$)$_3$ ($0 \le x \le 1$) of the archetypal (noncentrosymmetric) Kondo insulator Ce$_3$Bi$_4$Pt$_3$. The Pt-Pd substitution is isostructural, isoelectronic, and isosize, and therefore likely to leave $J_{\text{K}}$ and $μ$ essentially unchanged. By contrast, the large mass difference between the $5d$ element Pt and the $4d$ element Pd leads to a large difference in $λ_{\rm{SOC}}$, which thus is the dominating tuning parameter in the series. Surprisingly, with increasing $x$ (decreasing $λ_{\rm{SOC}}$), we observe a Kondo insulator to semimetal transition, demonstrating an unprecedented drastic influence of the SOC. The fully substituted end compound Ce$_3$Bi$_4$Pd$_3$ shows thermodynamic signatures of a recently predicted Weyl-Kondo semimetal.

cond-mat.str-el

Ce 3$p$ hard x-ray photoelectron spectroscopy study of the topological Kondo insulator CeRu$_4$Sn$_6$

Bulk sensitive hard x-ray photoelectron spectroscopy data of the Ce 3$p$ core level of CeRu$_4$Sn$_6$ are presented. Using a combination of full multiplet and configuration iteration model we were able to obtain an accurate lineshape analysis of the data, thereby taking into account correlations for the strong plasmon intensities. We conclude that CeRu$_4$Sn$_6$ is a moderately mixed valence compound with a weight of 8% for the Ce $f^0$ configuration in the ground state.

cond-mat.str-el