arXiv subjects

Philipp Gegenwart

Publications and source records attributed to Philipp Gegenwart.

At least 55 records · Page 3Linked to original sources

arXiv2022

Resolving structural changes and symmetry lowering in spinel FeCr2S4

The cubic spinel FeCr2S4 has been receiving immense research interest because of its emergent phases and the interplay of spin, orbital and lattice degrees of freedom. Despite the intense research, several fundamental questions are yet to be answered, such as the refinement of the crystal structure in the different magnetic and orbital ordered phases. Here, using high-resolution synchrotron powder diffraction on stoichiometric crystals of FeCr2S4 we resolved the long sought-after cubic to tetragonal transition at ~65 K, reducing the lattice symmetry to I41/amd. With further lowering the temperature, at ~9 K, the crystal structure becomes polar, hence the compound becomes multiferroic. The elucidation of the lattice symmetry throughout different phases of FeCr2S4 provides a basis for the understanding this enigmatic system and also highlights the importance of structural deformation in correlated materials.

cond-mat.mtrl-sci↗

arXiv2022

Pressure-induced dimerization and collapse of antiferromagnetism in the Kitaev material $α$-Li$_2$IrO$_3$

We present magnetization measurements carried out on polycrystalline and single-crystalline samples of $α$-Li$_2$IrO$_3$ under hydrostatic pressures up to 2 GPa and establish the temperature-pressure phase diagram of this material. The Néel temperature ($T_{\rm{N}}$) of $α$-Li$_2$IrO$_3$ is slightly enhanced upon compression with $dT_{\rm{N}}/dp$ = 1.5 K/GPa. Above 1.2 GPa, $α$-Li$_2$IrO$_3$ undergoes a first-order phase transition toward a nonmagnetic dimerized phase, with no traces of the magnetic phase observed above 1.8 GPa at low temperatures. The critical pressure of the structural dimerization is strongly temperature-dependent. This temperature dependence is well reproduced on the ab initio level by taking into account lower phonon entropy in the nonmagnetic phase. We further show that the initial increase in $T_{\rm{N}}$ of the magnetic phase is due to a weakening of the Kitaev interaction $K$ along with the enhancement of the Heisenberg term $J$ and off-diagonal anisotropy $Γ$. Our study reveals a common thread in the interplay of magnetism and dimerization in pressured Kitaev materials.

cond-mat.str-el↗

arXiv2021

Interplay of magnetism and dimerization in pressurized Kitaev material $β$-Li$_2$IrO$_3$

We present magnetization measurements on polycrystalline $β$-Li$_2$IrO$_3$ under hydrostatic pressures up to 3~GPa and construct the temperature-pressure phase diagram of this material. Our data confirm that magnetic order breaks down in a first-order phase transition at $p_{\rm{c}}$ $\approx$ 1.4~GPa and additionally reveal a step-like feature -- magnetic signature of structural dimerization -- that appears at $p_{\rm{c}}$ and shifts to higher temperatures upon further compression. Following the structural study by L. S. I. Veiga et al. [Phys. Rev. B 100, 064104 (2019)], we suggest that a partially dimerized phase with a mixture of magnetic and non-magnetic Ir$^{4+}$ sites develops above $p_{\rm{c}}$. This phase is thermodynamically stable between 1.7 and 2.7~GPa according to our ab initio calculations. It confines the magnetic Ir$^{4+}$ sites to weakly coupled tetramers with a singlet ground state and no long-range magnetic order. Our results rule out the formation of a pressure-induced spin-liquid phase in $β$-Li$_2$IrO$_3$ and reveal peculiarities of the magnetism collapse transition in a Kitaev material. We also show that a compressive strain imposed by the pressure treatment of $β$-Li$_2$IrO$_3$ enhances signatures of the 100~K magnetic anomaly at ambient pressure.

cond-mat.str-el↗

arXiv2021

Electronic reconstruction and charge transfer in strained Sr$_2$CoIrO$_6$ double perovskite

The electronic, magnetic and optical properties of the double perovskite Sr$_2$CoIrO$_6$ (SCIO) under biaxial strain are explored in the framework of density functional theory (DFT) including a Hubbard $U$ term and spin-orbit coupling (SOC) in combination with absorption spectroscopy measurements on epitaxial thin films. While the end member SrIrO$_3$ is a semimetal with a quenched spin and orbital moment and bulk SrCoO$_3$ is a ferromagnetic (FM) metal with spin and orbital moment of 2.50 and 0.13 $μ_{B}$, respectively, the double perovskite SCIO emerges as an antiferromagnetic Mott insulator with antiparallel alignment of Co, Ir planes along the [110]-direction. Co exhibits a spin and enhanced orbital moment of $\sim 2.35-2.45$ and $0.31-$0.45 $μ_{B}$, respectively. Most remarkably, Ir acquires a significant spin and orbital moment of 1.21-1.25 and 0.13 $μ_{B}$, respectively. Analysis of the orbital occupation indicates an electronic reconstruction due to a substantial charge transfer from minority to majority spin states in Ir and from Ir to Co, signaling an Ir$^{4+δ}$, Co$^{4-δ}$ configuration. Biaxial strain, varied from -1.02% ($a_{\rm NdGaO_3}$) through 0% ($a_{\rm SrTiO_3}$) to 1.53% ($a_{\rm GdScO_3}$), influences in partcular the orbital polarization of the $t_{2g}$ states and leads to a nonmonotonic change of the band gap between 163 and 235 meV. The absorption coefficient reveals a two plateau fearure due to transitions from the valence to the lower lying narrow $t_{2g}$ and the higher lying broader $e_{g}$ bands. Inclusion of many body effects, in particular, excitonic effects by solving the Bethe-Salpeter equation (BSE), increases the band gap by $\sim0.2$ and improves the agreement with the measured spectrum concerning the position of the second peak at $\sim 2.6$ eV.

cond-mat.str-el↗

arXiv2021

Kitaev magnetism through the prism of lithium iridate

Fifteen years since its inception, the Kitaev model still boasts only a narrow group of material realizations. We review the progress in studying and understanding one of them, lithium iridate Li$_2$IrO$_3$ available in three polymorphs that host strong Kitaev interactions on spin lattices of different dimensionality and topology. We also discuss feasibility, effectiveness, and repercussions of tuning strategies based on the application of external pressure and chemical substitutions.

cond-mat.str-el↗

arXiv2021

Angular dependence of Hall effect and magnetoresistance in SrRuO$_3$-SrIrO$_3$ heterostructures

Perovskite SrRuO$_3$ is a prototypical itinerant ferromagnet which allows interface engineering of its electronic and magnetic properties. We report synthesis and investigation of atomically flat artificial multilayers of SrRuO$_3$ with the spin-orbit semimetal SrIrO$_3$ in combination with band-structure calculations with a Hubbard $U$ term and topological analysis. They reveal an electronic reconstruction and emergence of flat Ru-4d$_{xz}$ bands near the interface, ferromagnetic interlayer coupling and negative Berry-curvature contribution to the anomalous Hall effect. We analyze the Hall effect and magnetoresistance measurements as a function of the field angle from out of plane towards in-plane orientation (either parallel or perpendicular to the current direction) by a two-channel model. The magnetic easy direction is tilted by about $20^\circ$ from the sample normal for low magnetic fields, rotating towards the out-of-plane direction by increasing fields. Fully strained epitaxial growth enables a strong anisotropy of magnetoresistance. An additional Hall effect contribution, not accounted for by the two-channel model is compatible with stable skyrmions only up to a critical angle of roughly $45^\circ$ from the sample normal. Within about $20^\circ$ from the thin film plane an additional peak-like contribution to the Hall effect suggests the formation of a non-trivial spin structure.

cond-mat.str-el↗

arXiv2020

Field evolution of the spin-liquid candidate YbMgGaO$_4$

We report magnetization, heat capacity, thermal expansion, and magnetostriction measurements down to millikelvin temperatures on the triangular antiferromagnet YbMgGaO$_4$. Our data exclude the formation of the distinct $\frac13$ plateau phase observed in other triangular antiferromagnets, but reveal plateaulike features in second derivatives of the free energy, magnetic susceptibility and specific heat, at $μ_0H$ = 1.0 - 2.5 T for $H\parallel{}c$ and 2 - 5 T for $H\perp{}c$. Using Monte-Carlo simulations of a realistic spin Hamiltonian, we ascribe these features to nonmonotonic changes in the magnetization and the $\frac12$ plateau that is smeared out by the random distribution of exchange couplings in YbMgGaO$_4$.

cond-mat.str-el↗

arXiv2020

Conductivity of Dirac-like surface states in correlated honeycomb transition metal oxide Mott insulators

The search for materials with novel and unusual electronic properties is at the heart of condensed matter physics as well as the basis to develop conceptual new technologies. In this context, the correlated honeycomb transition metal oxides attract large attention for both, being a possible experimental realization of the theoretically predicted magnetic Kitaev exchange and the theoretical prospect of topological nontriviality. The Mott insulating sodium iridate is prototypical among these materials with the promising prospect to bridge the field of strongly correlated systems with topology, finally opening a path to a wide band gap material with exotic surface properties. Here, we report a profound study of the electronic properties of ultra-high-vacuum cleaved surfaces combining transport measurements with scanning tunneling techniques, showing that multiple conductive channels with differing nature are simultaneously apparent in this material. Most importantly, a V-shaped density of states and a low sheet resistance, in spite of a large defect concentration, point towards a topologically protected surface conductivity contribution. By incorporating the issue of the addressability of electronic states in the tunneling process, we develop a framework connecting previous experimental results as well as theoretical considerations.

cond-mat.str-el↗

arXiv2020

Persistent spin dynamics in the pressurized spin-liquid candidate YbMgGaO$_4$

Single-crystal x-ray diffraction, density-functional band-structure calculations, and muon spin relaxation ($μ$SR) are used to probe pressure evolution of the triangular spin-liquid candidate YbMgGaO$_4$. The rhombohedral crystal structure is retained up to at least 10 GPa and shows a nearly uniform compression along both in-plane and out-of-plane directions, whereas local distortions caused by the random distribution of Mg$^{2+}$ and Ga$^{3+}$ remain mostly unchanged. The $μ$SR data confirm persistent spin dynamics up to 2.6 GPa and down to 250 mK with no change in the muon relaxation rate. Longitudinal-field $μ$SR reveals power-law behavior of the spin-spin autocorrelation function, both at ambient pressure and upon compression.

cond-mat.str-el↗

arXiv2020

Soft and anisotropic local moments in 4$d$ and 5$d$ mixed-valence M$_2$O$_9$ dimers

We investigate via exact diagonalization of finite clusters the electronic structure and magnetism of M$_2$O$_9$ dimers in the mixed-valence hexagonal perovskites A$_3$B'M$_2$O$_9$ for various different fillings of 4$d$ and 5$d$ transition-metal M ions. We find that the magnetic moments of such dimers are determined by a subtle interplay of spin-orbit coupling, Hund's coupling, and Coulomb repulsion, as well as the electron filling of the M ions. Most importantly, the magnetic moments are anisotropic and temperature-dependent. This behavior is a result of spin-orbit coupling, magnetic field effects, and the existence of several nearly-degenerate electronic configurations whose proximity allows occupation of excited states already at room temperature. This analysis is consistent with experimental susceptibility measurements for a variety of dimer-based materials. Furthermore, we perform a survey of A$_3$B'M$_2$O$_9$ materials and propose ground-state phase diagrams for the experimentally relevant M fillings of $d^{4.5}$, $d^{3.5}$ and $d^{2.5}$. Finally, our results show that the usually applied Curie-Weiss law with a constant magnetic moment cannot be used in these spin-orbit-coupled materials.

cond-mat.str-el↗

arXiv2020

Realization of the kagome spin ice state in a frustrated intermetallic compound

Spin ices are exotic phases of matter characterized by frustrated spins obeying local ice rules, in analogy with the electric dipoles in water ice. In two dimensions, one can similarly define ice rules for in-plane Ising-like spins arranged on a kagome lattice. These ice rules require each triangle plaquette to have a single monopole, and can lead to various unique orders and excitations. Using experimental and theoretical approaches including magnetometry, thermodynamic measurements, neutron scattering and Monte Carlo simulations, we establish HoAgGe as a crystalline (i.e. non-artificial) system that realizes the kagome spin ice state. The system features a variety of partially and fully ordered states and a sequence of field-induced phases at low temperatures, all consistent with the kagome ice rule.

cond-mat.str-el↗

arXiv2020

Spin liquids in geometrically perfect triangular antiferromagnets

The cradle of quantum spin liquids, triangular antiferromagnets show strong proclivity to magnetic order and require deliberate tuning to stabilize a spin-liquid state. In this brief review, we juxtapose recent theoretical developments that trace the parameter regime of the spin-liquid phase, with experimental results for Co-based and Yb-based triangular antiferromagnets. Unconventional spin dynamics arising from both ordered and disordered ground states is discussed, and the notion of a geometrically perfect triangular system is scrutinized to demonstrate non-trivial imperfections that may assist magnetic frustration in stabilizing dynamic spin states with peculiar excitations.

cond-mat.str-el↗

arXiv2019

Magnetic frustration in a metallic fcc lattice

Magnetic frustration in metals is scarce and hard to pinpoint, but exciting due to the possibility of the emergence of fascinating novel phases. The cubic intermetallic compound HoInCu$_4$ with all holmium atoms on an fcc lattice, exhibits partial magnetic frustration, yielding a ground state where half of the Ho moments remain without long-range order, as evidenced by our neutron scattering experiments. The substitution of In with Cd results in HoCdCu$_4$ in a full breakdown of magnetic frustration. Consequently we found a fully ordered magnetic structure in our neutron diffraction experiments. These findings are in agreement with the local energy scales and crystal electric field excitations, which we determined from specific heat and inelastic neutron scattering data. The electronic density of states for the itinerant bands acts as tuning parameter for the ratio between nearest-neighbor and next-nearest-neighbor interactions and thus for magnetic frustration.

cond-mat.str-el↗

arXiv2019

Quantum-critical phase out of frustrated magnetism in a strongly correlated metal

Strange-metal phenomena often develop at the border of antiferromagnetic order in strongly correlated metals. It has been well established that they can originate from the fluctuations anchored by the point of continuous quantum phase transition out of the antiferromagnetic order, i.e., a quantum critical point. What has been unclear is how these phenomena can be associated with a potential new phase of matter at zero temperature. Here we show that magnetic frustration of the 4f-local moments in the distorted Kagome intermetallic compound CePdAl gives rise to such a paramagnetic quantum-critical phase. Moreover, we demonstrate that this phase turns into a Fermi liquid through a Mott-like crossover; in a two-dimensional parameter space of pressure and magnetic field, this crossover is linked to a line of zero-temperature 4f-electron localization-delocalization phase transitions at low and moderate pressures. Our discovery motivates a new design principle for strongly correlated metallic states with unconventional excitations that may underlie the development of such effects as high temperature superconductivity.

cond-mat.str-el↗

arXiv2019

Rearrangement of uncorrelated valence bonds evidenced by low-energy spin excitations in YbMgGaO4

DC-magnetization data measured down to 40 mK speak against conventional freezing and reinstate YbMgGaO$_4$ as a triangular spin-liquid candidate. Magnetic susceptibility measured parallel and perpendicular to the $c$-axis reaches constant values below 0.1 and 0.2 K, respectively, thus indicating the presence of gapless low-energy spin excitations. We elucidate their nature in the triple-axis inelastic neutron scattering experiment that pinpoints the low-energy ($E$ $\leq$ $J_0$ $\sim$ 0.2 meV) part of the excitation continuum present at low temperatures ($T$ $<$ $J_0$/$k_B$), but \emph{completely} disappearing upon warming the system above $T$ $\gg$ $J_0$/$k_B$. In contrast to the high-energy part at $E$ $>$ $J_0$ that is rooted in the breaking of nearest-neighbor valence bonds and persists to temperatures well above $J_0$/$k_B$, the low-energy one originates from the rearrangement of the valence bonds and thus from the propagation of unpaired spins. We further extend this picture to herbertsmithite, the spin-liquid candidate on the kagome lattice, and argue that such a hierarchy of magnetic excitations may be a universal feature of quantum spin liquids.

cond-mat.str-el↗

arXiv2019

Gapless spin-liquid state in the structurally disorder-free triangular antiferromagnet NaYbO$_2$

We present the structural characterization and low-temperature magnetism of the triangular-lattice delafossite NaYbO$_2$. Synchrotron x-ray diffraction and neutron scattering exclude both structural disorder and crystal-electric-field randomness, whereas heat-capacity measurements and muon spectroscopy reveal the absence of magnetic order and persistent spin dynamics down to at least 70\,mK. Continuous magnetic excitations with the low-energy spectral weight accumulating at the $K$-point of the Brillouin zone indicate the formation of a novel spin-liquid phase in a triangular antiferromagnet. This phase is gapless and shows a non-trivial evolution of the low-temperature specific heat. Our work demonstrates that NaYbO$_2$ practically gives the most direct experimental access to the spin-liquid physics of triangular antiferromagnets.

cond-mat.str-el↗

arXiv2018

Investigation of Thermodynamic Properties of Cu(NH3)4SO4.H2O, a Heisenberg Spin Chain Compound

Detailed experimental investigations of thermal and magnetic properties are presented for Cu(NH3)4SO4.H2O, an ideal uniform Heisenberg spin half chain compound. A comparison of these properties with relevant spin models is also presented. The temperature dependent magnetic susceptibility and specific heat data has been compared with the exact solution for uniform Heisenberg chain model derived by means of Bethe ansatz technique. Field dependent isothermal magnetization curves are simulated by Quantum Monte Carlo technique and compared with the corresponding experimental ones. Specific heat as a function of magnetic field (up to 7T) and temperature (down to 2K) is reported. Subsequently, the data are compared with the corresponding theoretical curves for the infinite Heisenberg spin half chain model with J=6K. Moreover, internal energy and entropy are calculated by analyzing the experimental specific heat data. Magnetic field and temperature dependent behavior of entropy and internal energy are in good agreement with the theoretical predictions.

cond-mat.str-el↗

arXiv2018

Observation of two critical points linked to the high field phase B in CeCu2Si2

We present thermal expansion and magnetostriction measurements on a CeCu2Si2 single crystal of A/S-type up to 17.9T magnetic field applied along the crystallographic a-direction (Delta L ll a ll H) and down to 0.015K temperature. We identify clear thermodynamic anomalies at the superconducting transition T_c and at two second order transitions T_A,B into ordered phases A and B. Our measurements establish for the first time the boundary of phase B at high field and low temperature. No evidence for additional high field phases above B is found up to the maximum field. We speculate based on our experimental results that i) phase B is similar to phase A of spin-density wave type and ii) the first order phase transition between A and B is caused by Fermi surface reconstruction. We furthermore identify a new quantum critical point at H_c ~ 17T, where T_B is suppresssed to zero, and a bicritical point at (0.35K, 7.0T), where phase lines T_A(H) and T_B(H) meet.

cond-mat.str-el↗