arXiv subjects

P. Gegenwart

Publications and source records attributed to P. Gegenwart.

At least 55 records · Page 3Linked to original sources

arXiv2018

Spin dynamics and field-induced magnetic phase transition in the honeycomb Kitaev magnet $α$-Li$_2$IrO$_3$

The layered honeycomb iridate $α$-Li$_2$IrO$_3$ displays an incommensurate magnetic structure with counterrotating moments on nearest-neighbor sites, proposed to be stabilized by strongly-frustrated anisotropic Kitaev interactions between spin-orbit entangled Ir$^{4+}$ magnetic moments. Here we report powder inelastic neutron scattering measurements that observe sharply dispersive low-energy magnetic excitations centered at the magnetic ordering wavevector, attributed to Goldstone excitations of the incommensurate order, as well as an additional intense mode above a gap $Δ\simeq2.3$ meV. Zero-field muon-spin relaxation measurements show clear oscillations in the muon polarization below the Néel temperature $T_{\rm N}\simeq15$ K with a time-dependent profile consistent with bulk incommensurate long-range magnetism. Pulsed field magnetization measurements observe that only about half the saturation magnetization value is reached at the maximum field of 64 T. A clear anomaly near 25 T indicates a transition to a phase with reduced susceptibility. The transition field has a Zeeman energy comparable to the zero-field gapped mode, suggesting gap suppression as a possible mechanism for the field-induced transition.

cond-mat.str-el↗

arXiv2018

Breakdown of magnetic order in the pressurized Kitaev iridate $β$-Li$_2$IrO$_3$

Temperature-pressure phase diagram of the Kitaev hyperhoneycomb iridate $β$-Li$_2$IrO$_3$ is explored using magnetization, thermal expansion, magnetostriction, and muon spin rotation ($μ$SR) measurements, as well as single-crystal x-ray diffraction under pressure and ab initio calculations. The Neel temperature of $β$-Li$_2$IrO$_3$ increases with the slope of 0.9 K/GPa upon initial compression, but the reduction in the polarization field $H_c$ reflects a growing instability of the incommensurate order. At 1.4 GPa, the ordered state breaks down upon a first-order transition giving way to a new ground state marked by the coexistence of dynamically correlated and frozen spins. This partial freezing in the absence of any conspicuous structural defects may indicate classical nature of the resulting pressure-induced spin liquid, an observation paralleled to the increase in the nearest-neighbor off-diagonal exchange $Γ$ under pressure.

cond-mat.str-el↗

arXiv2018

Fully gapped $d$-wave superconductivity in CeCu$_2$Si$_2$

The nature of the pairing symmetry of the first heavy fermion superconductor CeCu$_2$Si$_2$ has recently become the subject of controversy. While CeCu$_2$Si$_2$ was generally believed to be a $d$-wave superconductor, recent low temperature specific heat measurements showed evidence for fully gapped superconductivity, contrary to the nodal behavior inferred from earlier results. Here we report London penetration depth measurements, which also reveal fully gapped behavior at very low temperatures. To explain these seemingly conflicting results, we propose a fully gapped $d+d$ band-mixing pairing state for CeCu$_2$Si$_2$, which yields very good fits to both the superfluid density and specific heat, as well as accounting for a sign change of the superconducting order parameter, as previously concluded from inelastic neutron scattering results.

cond-mat.supr-con↗

arXiv2018

Strain induced changes of electronic properties of B-site ordered double perovskite Sr$_2$CoIrO$_6$ thin films

B-site ordered thin films of double perovskite Sr$_2$CoIrO$_6$ were epitaxially grown by a metal-organic aerosol deposition technique on various substrates, actuating different strain states. X-ray diffraction, transmission electron microscopy and polarized far-field Raman spectroscopy confirm the strained epitaxial growth on all used substrates. Polarization dependent Co $L_{2,3}$ X-ray absorption spectroscopy reveals a change of the magnetic easy axis of the antiferromagnetically ordered (high-spin) Co$^{3+}$ sublattice within the strain series. By reversing the applied strain direction from tensile to compressive, the easy axis changes abruptly from in-plane to out-of-plane orientation. The low-temperature magnetoresistance changes its sign respectively and is described by a combination of weak anti-localization and anisotropic magnetoresistance effects.

cond-mat.str-el↗

arXiv2018

Quantum oscillations and Dirac dispersion in the BaZnBi2 semimetal guaranteed by local Zn vacancy order

We have synthesized single crystals of Dirac semimetal candidates AZnBi2 with A=Ba and Sr. In contrast to A=Sr, the Ba material displays a novel local Zn vacancy ordering, which makes the observation of quantum oscillations in out-of-plane magnetic fields possible. As a new Dirac semimetal candidate, BaZnBi2 exhibits small cyclotron electron mass, high quantum mobility, and non-trivial Berry phases. Three Dirac dispersions are observed by ARPES and identified by first- principles band-structure calculations. Compared to AMn(Bi/Sb)2 systems which host Mn magnetic moments, BaZnBi2 acts as non-magnetic analogue to investigate the intrinsic properties of Dirac fermions in this structure family.

cond-mat.str-el↗

arXiv2018

Discovery of Emergent Photon and Monopoles in a Quantum Spin Liquid

Quantum spin liquid (QSL) is an exotic quantum phase of matter whose ground state is quantum-mechanically entangled without any magnetic ordering. A central issue concerns emergent excitations that characterize QSLs, which are hypothetically associated with quasiparticle fractionalization and topological order. Here we report highly unusual heat conduction generated by the spin degrees of freedom in a QSL state of the pyrochlore magnet Pr$_2$Zr$_2$O$_7$, which hosts spin-ice correlations with strong quantum fluctuations. The thermal conductivity in high temperature regime exhibits a two-gap behavior, which is consistent with the gapped excitations of magnetic ($M$-) and electric monopoles ($E$-particles). At very low temperatures below 200\,mK, the thermal conductivity unexpectedly shows a dramatic enhancement, which well exceeds purely phononic conductivity, demonstrating the presence of highly mobile spin excitations. This new type of excitations can be attributed to emergent photons ($ν$-particle), coherent gapless spin excitations in a spin-ice manifold.

cond-mat.str-el↗

arXiv2017

Uniaxial stress tuning of geometrical frustration in a Kondo lattice

Hexagonal CeRhSn with paramagnetic $4f$ moments on a distorted Kagome lattice displays zero-field quantum critical behavior related to geometrical frustration. We report high-resolution thermal expansion and magnetostriction measurements under multiextreme conditions such as uniaxial stress up to 200 MPa, temperatures down to 0.1 K and magnetic fields up to 10 T. Under uniaxial stress along the $a$-direction, quantum criticality disappears and a complex magnetic phase diagram arises with a sequence of phases below 1.2 K and fields between 0 and 3 T ($\parallel a$). Since the Kondo coupling increases with stress, which alone would stabilize paramagnetic behavior in CeRhSn, the observed order arises from the release of geometrical frustration by in-plane stress.

cond-mat.str-el↗

arXiv2017

Competition between spin-orbit coupling, magnetism, and dimerization in the honeycomb iridates: $α$-Li$_{2}$IrO$_{3}$ under pressure

Single-crystal x-ray diffraction studies with synchrotron radiation on the honeycomb iridate $α$-Li$_{2}$IrO$_{3}$ reveal a pressure-induced structural phase transition with symmetry lowering from monoclinic to triclinic at a critical pressure of $P_{c}$ = 3.8 GPa. According to the evolution of the lattice parameters with pressure, the transition mainly affects the $ab$ plane and thereby the Ir hexagon network, leading to the formation of Ir--Ir dimers. These observations are independently predicted and corroborated by our \textit{ab initio} density functional theory calculations where we find that the appearance of Ir--Ir dimers at finite pressure is a consequence of a subtle interplay between magnetism, correlation, spin-orbit coupling, and covalent bonding. Our results further suggest that at $P_{c}$ the system undergoes a magnetic collapse. Finally we provide a general picture of competing interactions for the honeycomb lattices $A_{2}$$M$O$_{3}$ with $A$= Li, Na and $M$ = Ir, Ru.

cond-mat.str-el↗

arXiv2017

Persistent low-temperature spin dynamics in the mixed-valence iridate Ba$_{3}$InIr$_{2}$O$_{9}$

Using thermodynamic measurements, neutron diffraction, nuclear magnetic resonance, and muon spin relaxation, we establish putative quantum spin-liquid behavior in Ba$_3$InIr$_2$O$_9$, where unpaired electrons are localized on mixed-valence Ir$_2$O$_9$ dimers with Ir$^{4.5+}$ ions. Despite the antiferromagnetic Curie-Weiss temperature on the order of 10 K, neither long-range magnetic order nor spin freezing are observed down to at least 20 mK, such that spins are short-range correlated and dynamic over nearly three decades in temperature. Quadratic power-law behavior of both the spin-lattice relaxation rate and specific heat indicates the gapless nature of the ground state. We envisage that this exotic behavior may be related to an unprecedented combination of the triangular and buckled honeycomb geometries of nearest-neighbor exchange couplings in the mixed-valence setting.

cond-mat.str-el↗

arXiv2017

High-pressure versus isoelectronic doping effect on the honeycomb iridate Na$_2$IrO$_3$

We study the effect of isoelectronic doping and external pressure in tuning the ground state of the honeycomb iridate Na$_2$IrO$_3$ by combining optical spectroscopy with synchrotron x-ray diffraction measurements on single crystals. The obtained optical conductivity of Na$_2$IrO$_3$ is discussed in terms of a Mott insulating picture versus the formation of quasimolecular orbitals and in terms of Kitaev-interactions. With increasing Li content $x$, (Na$_{1-x}$Li$_x$)$_2$IrO$_3$ moves deeper into the Mott insulating regime and there are indications that up to a doping level of 24\% the compound comes closer to the Kitaev-limit. The optical conductivity spectrum of single crystalline $α$-Li$_2$IrO$_3$ does not follow the trends observed for the series up to $x=0.24$. There are strong indications that $α$-Li$_2$IrO$_3$ is less close to the Kitaev-limit compared to Na$_2$IrO$_3$ and closer to the quasimolecular orbital picture. Except for the pressure-induced hardening of the phonon modes, the optical properties of Na$_2$IrO$_3$ seem to be robust against external pressure. Possible explanations of the unexpected evolution of the optical conductivity with isolectronic doping and the drastic change between $x=0.24$ and $x=1$ are given by comparing the pressure-induced changes of lattice parameters and the optical conductivity with the corresponding changes induced by doping.

cond-mat.str-el↗

arXiv2017

Local Magnetism and Spin Dynamics of the Frustrated Honeycomb Rhodate Li2RhO3

We report magnetization, heat capacity, 7Li - nuclear magnetic resonance (NMR), and muSR (muon spin roration) measurements on the honeycomb 4d5 spin liquid candidate Li2RhO3. The magnetization in small magnetic fields provides evidence of the partial spin-freezing of a small fraction of Rh4+ -moments at 6 K, whereas the Curie-Weiss behavior above 100 K suggests a pseudo-spin-1/2 paramagnet with a moment of about 2.2 muB. The magnetic specific heat (Cm) exhibits no field dependence and demonstrates the absence of long range magnetic order down to 0.35 K. Cm/T passes through a broad maximum at about 10 K and Cm=T^2 at low temperatures. Measurements of the spin-lattice relaxation rate (1/T1) reveal a gapless slowing down of spin fluctuations upon cooling with 1/T1=T^2.2. The results from NMR and muSR are consistent with a scenario in which a minority of Rh4+ moments are in a ahort-range correlated frozen state and coexist with a majority of moments in a liquid-like state that continue to fluctuate at low temperatures.

cond-mat.str-el↗

arXiv2017

The collapsed tetragonal phase as a strongly covalent and fully nonmagnetic state: persistent magnetism with interlayer As-As bond formation in Rh-doped Ca$_{0.8}$Sr$_{0.2}$Fe$_2$As$_2$

A well-known feature of CaFe$_{2}$As$_{2}$-based superconductors is the pressure-induced collapsed tetragonal phase that is commonly ascribed to the formation of an interlayer As-As bond. Using detailed X-ray scattering and spectroscopy, we find that Rh-doped Ca$_{0.8}$Sr$_{0.2}$Fe$_{2}$As$_{2}$ does not undergo a first-order phase transition and that local Fe moments persist despite the formation of interlayer As-As bonds. Our density functional theory calculations reveal that the Fe-As bond geometry is critical for stabilizing magnetism and that the pressure-induced drop in the $c$ lattice parameter observed in pure CaFe$_{2}$As$_{2}$ is mostly due to a constriction within the FeAs planes. These phenomena are best understood using an often overlooked explanation for the equilibrium Fe-As bond geometry, which is set by a competition between covalent bonding and exchange splitting between strongly hybridized Fe $3d$ and As $4p$ states. In this framework, the collapsed tetragonal phase emerges when covalent bonding completely wins out over exchange splitting. Thus the collapsed tetragonal phase is properly understood as a strong, covalent phase that is fully nonmagnetic with the As-As bond forming as a byproduct.

cond-mat.str-el↗

arXiv2016

Single crystal growth from separated educts and its application to lithium transition-metal oxides

Thorough mixing of the starting materials is the first step of a crystal growth procedure. This holds true for almost any standard technique, whereas the intentional separation of educts is considered to be restricted to a very limited number of cases. A noticeable exception is the crystal growth in gels that allows for a better control of the nucleation by limiting the diffusion. The successful application of this principle to open systems, however, has remained elusive. Here we show that single crystals of α-Li2IrO3 can be grown from separated educts in an open crucible in air. Elemental lithium and iridium are oxidized and transported over a distance of typically one centimeter in an isothermal process. Single crystals grow from an exposed condensation point placed in between the educts. The method has also been applied to the growth of Li2RuO3, Li2PtO3 and β-Li2IrO3 and a successful use for various other materials is anticipated.

cond-mat.mtrl-sci↗

arXiv2016

Experimental evidence for the importance of Hund's exchange interaction for the incoherence of the charge carriers in iron-based superconductors

Angle-resolved photoemission spectroscopy (ARPES) is used to study the scattering rates of charge carriers from the hole pockets near Gamma in the iron-based high-Tc hole doped superconductors KxBa1-xFe2As2 x=0.4 and KxEu1-xFe2As2 x=0.55$ and the electron doped compound Ba(Fe1-xCox)2As2 x=0.075. The scattering rate for any given band is found to depend linearly on energy, indicating a non-Fermi liquid regime. The scattering rates in the hole-doped compound are considerably larger than those in the electron-doped compounds. In the hole-doped systems the scattering rate of the charge carriers of the inner hole pocket is about three times bigger than the binding energy indicating that the spectral weight is heavily incoherent. The strength of the scattering rates and the difference between electron and hole doped compounds signals the importance of Hund's exchange coupling for correlation effects in these iron-based high-Tc superconductors. The experimental results are in qualitative agreement with theoretical calculations in the framework of combined density functional dynamical mean-field theory.

cond-mat.supr-con↗

arXiv2016

Bose glass behavior in (Yb$_{1-x}$Lu$_x$)$_4$As$_3$ representing the randomly diluted quantum spin-1/2 chains

The site-diluted compound (Yb$_{1-x}$Lu$_x$)$_4$As$_3$ is a scarce realization of the linear Heisenberg antiferromagnet partitioned into finite-size segments and is an ideal model compound for studying field-dependent effects of quenched disorder in the one-dimensional antiferromagnets. It differentiates from the systems studied so far in two aspects - the type of randomness and the nature of the energy gap in the pure sample. We have measured the specific heat of single-crystal (Yb$_{1-x}$Lu$_x$)$_4$As$_3$ in magnetic fields up to 19.5 T. The contribution $C_{\perp}$ arising from the magnetic subsystem in an applied magnetic field perpendicular to the chains is determined. Compared to pure Yb$_4$As$_3$, for which $C_{\perp}$ indicates a gap opening, for diluted systems a non-exponential decay is found at low temperatures which is consistent with the thermodynamic scaling of the specific heat established for a Bose-glass phase.

cond-mat.str-el↗

arXiv2016

A uniaxial stress capacitive dilatometer for high-resolution thermal expansion and magnetostriction under multiextreme conditions

Thermal expansion and magnetostriction are directional dependent thermodynamic quantities. For the characterization of novel quantum phases of matter it is required to study materials under multi-extreme conditions, in particular down to very low temperatures, in very high magnetic fields, as well as under high pressure. We developed a miniaturized capacitive dilatometer suitable for temperatures down to 20 mK and usage in high magnetic fields, which exerts a large spring force between 40 to 75 N on the sample. This corresponds to a uniaxial stress up to 3 kbar for a sample with cross-section of (0.5~mm)$^2$. We describe the design and performance test of the dilatometer which resolves length changes with high resolution of $0.02 \mathrmÅ$ at low temperatures. The miniaturized device can be utilized in any standard cryostat, including dilution refrigerators or the commercial physical property measurement system.

cond-mat.str-el↗

arXiv2016

Super-heavy fermion material as metallic refrigerant for adiabatic demagnetization cooling

Low-temperature refrigeration is of crucial importance in fundamental research of condensed matter physics, as the investigations of fascinating quantum phenomena, such as superconductivity, superfluidity and quantum criticality, often require refrigeration down to very low temperatures. Currently, cryogenic refrigerators with $^3$He gas are widely used for cooling below 1 Kelvin. However, usage of the gas is being increasingly difficult due to the current world-wide shortage. Therefore, it is important to consider alternative methods of refrigeration. Here, we show that a new type of refrigerant, super-heavy electron metal, YbCo$_2$Zn$_{20}$, can be used for adiabatic demagnetization refrigeration, which does not require 3He gas. A number of advantages includes much better metallic thermal conductivity compared to the conventional insulating refrigerants. We also demonstrate that the cooling performance is optimized in Yb$_{1-x}$Sc$_x$Co$_2$Zn$_{20}$ by partial Sc substitution with $x\sim$0.19. The substitution induces chemical pressure which drives the materials close to a zero-field quantum critical point. This leads to an additional enhancement of the magnetocaloric effect in low fields and low temperatures enabling final temperatures well below 100 mK. Such performance has up to now been restricted to insulators. Since nearly a century the same principle of using local magnetic moments has been applied for adiabatic demagnetization cooling. This study opens new possibilities of using itinerant magnetic moments for the cryogen-free refrigeration.

cond-mat.str-el↗

arXiv2016

T/B scaling without quasiparticle mass divergence: YbCo2Ge4

YbCo$_2$Ge$_4$ is a clean paramagnetic Kondo lattice which displays non-Fermi liquid behavior. We report a detailed investigation of the specific heat, magnetic Grüneisen parameter ($Γ_{\rm mag}$) and temperature derivative of the magnetization ($M$) on a high-quality single crystal at temperatures down to $0.1$~K and magnetic fields up to 7~T. $Γ_{\rm mag}$ and $dM/dT$ display a divergence upon cooling and obey $T/B$ scaling. Similar behavior has previously been found in several other Yb-based Kondo lattices and related to a zero-field quantum critical point without fine tuning of pressure or composition. However, in the approach of $B\rightarrow 0$ the electronic heat capacity coefficient of YbCo$_2$Ge$_4$ saturates at low $T$, excluding ferromagnetic quantum criticality. This indicates that $T/B$ scaling is insufficient to prove a zero-field quantum critical point.

cond-mat.str-el↗