arXiv subjects

J. van den Brink

Publications and source records attributed to J. van den Brink.

At least 37 records · Page 2Linked to original sources

arXiv2019

Fingerprints of Kitaev physics in the magnetic excitations of honeycomb iridates

In the quest for realizations of quantum spin liquids, the exploration of Kitaev materials - spin-orbit entangled Mott insulators with strong bond-directional exchanges - has taken center stage. However, in these materials the local spin-orbital j=1/2 moments typically show long-range magnetic order at low temperature, thus defying the formation of a spin-liquid ground state. Using resonant inelastic x-ray scattering (RIXS), we here report on a proximate spin liquid regime with clear fingerprints of Kitaev physics in the magnetic excitations of the honeycomb iridates alpha-Li2IrO3 and Na2IrO3. We observe a broad continuum of magnetic excitations that persists up to at least 300K, more than an order of magnitude larger than the magnetic ordering temperatures. We prove the magnetic character of this continuum by an analysis of the resonance behavior. RIXS measurements of the dynamical structure factor for energies within the continuum show that dynamical spin-spin correlations are restricted to nearest neighbors. Notably, these spectroscopic observations are also present in the magnetically ordered state for excitation energies above the conventional magnon excitations. Phenomenologically, our data agree with inelastic neutron scattering results on the related honeycomb compound RuCl3, establishing a common ground for a proximate Kitaev spin-liquid regime in these materials.

cond-mat.str-el↗

arXiv2019

Magnetic anisotropy and spin-polarized two-dimensional electron gas in the van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$

We report a comprehensive experimental investigation on the magnetic anisotropy in bulk single crystals of Cr$_2$Ge$_2$Te$_6$, a quasi-two-dimensional ferromagnet belonging to the family of magnetic layered transition metal trichalcogenides that have attracted recently a big deal of interest with regard to the fundamental and applied aspects of two-dimensional magnetism. For this purpose electron spin resonance (ESR) and ferromagnetic resonance (FMR) measurements have been carried out over a wide frequency and temperature range. A gradual change in the angular dependence of the ESR linewidth at temperatures above the ferromagnetic transition temperature $T_{\rm c}$ reveals the development of two-dimensional spin correlations in the vicinity of $T_{\rm c}$ thereby proving the intrinsically low-dimensional character of spin dynamics in Cr$_2$Ge$_2$Te$_6$. Angular and frequency dependent measurements in the ferromagnetic phase clearly show an easy-axis type anisotropy of this compound. Furthermore, these experiments are compared with simulations based on a phenomenological approach, which takes into account results of static magnetization measurements as well as high temperature $g$ factors obtained from ESR spectroscopy in the paramagnetic phase. As a result the determined magnetocrystalline anisotropy energy density (MAE) $K_U$ is $(0.48 \pm 0.02) \times10^6$ erg/cm$^3$. This analysis is complemented by density functional calculations which yield the experimental MAE value for a particular value of the electronic correlation strength $U$. The analysis of the electronic structure reveals that the low-lying conduction band carries almost completely spin-polarized, quasi-homogeneous, two-dimensional states.

cond-mat.str-el↗

arXiv2019

Crossover from itinerant to localized magnetic excitations through the metal-insulator transition in NaOsO$_{\text{3}}$

NaOsO$_{\text{3}}$ undergoes a metal-insulator transition (MIT) at 410 K, concomitant with the onset of antiferromagnetic order. The excitation spectra have been investigated through the MIT by resonant inelastic x-ray scattering (RIXS) at the Os L$_{\text{3}}$ edge. Low resolution ($ΔE \sim$ 300 meV) measurements over a wide range of energies reveal that local electronic excitations do not change appreciably through the MIT. This is consistent with a picture in which structural distortions do not drive the MIT. In contrast, high resolution ($ΔE \sim $ 56 meV) measurements show that the well-defined, low energy magnons in the insulating state weaken and dampen upon approaching the metallic state. Concomitantly, a broad continuum of excitations develops which is well described by the magnetic fluctuations of a nearly antiferromagnetic Fermi liquid. By revealing the continuous evolution of the magnetic quasiparticle spectrum as it changes its character from itinerant to localized, our results provide unprecedented insight into the nature of the MIT in \naoso. In particular, the presence of weak correlations in the paramagnetic phase implies a degree of departure from the ideal Slater limit.

cond-mat.str-el↗

arXiv2019

Resonant inelastic x-ray incarnation of Young's double-slit experiment

Young's archetypal double-slit experiment forms the basis for modern diffraction techniques: the elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young's experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with structural Ir dimers and strong spin-orbit coupling. The double 'slits' in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures.

cond-mat.str-el↗

arXiv2018

An anomalous higher-order topological insulator

Topological multipole insulators are a class of higher order topological insulators (HOTI) in which robust fractional corner charges appear due to a quantized electric multipole moment of the bulk. This bulk-corner correspondence has been expressed in terms of a topological invariant computed using the eigenstates of the Wilson loop operator, a so called "nested Wilson loop" procedure. We show that, similar to the unitary Floquet operator describing periodically driven systems, the unitary Wilson loop operator can realize "anomalous" phases, that are topologically non-trivial despite having a trivial topological invariant. We introduce a concrete example of an anomalous HOTI, which has a quantized bulk quadrupole moment and fractional corner charges, but a vanishing nested Wilson loop index. A new invariant able to capture the topology of this phase is then constructed. Our work shows that anomalous topological phases, previously thought to be unique to periodically driven systems, can occur and be used to understand purely time-independent HOTIs.

cond-mat.mes-hall↗

arXiv2018

NaYbS$_2$ - a new planar spin-$\frac{1}{2}$ triangular-lattice magnet and putative spin liquid

Platelike high-quality NaYbS$_{2}$ rhombohedral single crystals with lateral dimensions of a few mm have been grown and investigated in great detail by bulk methods like magnetization and specific heat, but also by local probes like nuclear magnetic resonance (NMR), electron-spin resonance (ESR), muon-spin relaxation ($μ$SR), and inelastic neutron scattering (INS) over a wide field and temperature range. Our single-crystal studies clearly evidence a strongly anisotropic quasi-2D magnetism and an emerging spin-orbit entangled $S=1/2$ state of Yb towards low temperatures together with an absence of long-range magnetic order down to 260~mK. In particular, the clear and narrow Yb ESR lines together with narrow $^{23}$Na NMR lines evidence an absence of inherent structural distortions in the system, which is in strong contrast to the related spin-liquid candidate YbMgGaO$_{4}$ falling within the same space group $R\overline{3}m$. This identifies NaYbS$_{2}$ as a rather pure spin-1/2 triangular lattice magnet and a new putative quantum spin liquid.

cond-mat.str-el↗

arXiv2018

Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet alpha-RuCl3

Magnetization and high-resolution x-ray diffraction measurements of the Kitaev-Heisenberg material alpha-RuCl3 reveal a pressure-induced crystallographic and magnetic phase transition at a hydrostatic pressure of p=0.2 GPa. This structural transition into a triclinic phase is characterized by a very strong dimerization of the Ru-Ru bonds, accompanied by a collapse of the magnetic susceptibility. Ab initio quantum-chemistry calculations disclose a pressure-induced enhancement of the direct 4d-4d bonding on particular Ru-Ru links, causing a sharp increase of the antiferromagnetic exchange interactions. These combined experimental and computational data show that the Kitaev spin liquid phase in alpha-RuCl3 strongly competes with the crystallization of spin singlets into a valence bond solid.

cond-mat.str-el↗

arXiv2018

Nematicity and magnetism in LaFeAsO single crystals probed by $^{75}$As nuclear magnetic resonance

We report a $^{75}$As nuclear magnetic resonance study in LaFeAsO single crystals, which undergoes nematic and antiferromagnetic transitions at $T_\text{nem}\sim 156$ K and $T_N \sim 138$ K, respectively. Below $T_\text{nem}$, the $^{75}$As spectrum splits sharply into two for an external magnetic field parallel to the orthorhombic $a$ or $b$ axis in the FeAs planes. Our analysis of the data demonstrates that the NMR line splitting arises from an electronically driven rotational symmetry breaking. The $^{75}$As spin-lattice relaxation rate as a function of temperature shows that spin fluctuations are strongly enhanced just below $T_\text{nem}$. These NMR findings indicate that nematic order promotes spin fluctuations in magnetically ordered LaFeAsO, as observed in non-magnetic and superconducting FeSe. We conclude that the origin of nematicity is identical in both FeSe and LaFeAsO regardless of whether or not a long range magnetic order develops in the nematic state.

cond-mat.str-el↗

arXiv2018

Pressure-driven collapse of the relativistic electronic ground state in a honeycomb iridate

The electronic ground state in many iridate materials is described by a complex wave-function in which spin and orbital angular momenta are entangled due to relativistic spin-orbit coupling (SOC). Such a localized electronic state carries an effective total angular momentum of $J_{eff}=1/2$. In materials with an edge-sharing octahedral crystal structure, such as the honeycomb iridates Li2IrO3 and Na2IrO3, these $J_{eff}=1/2$ moments are expected to be coupled through a special bond-dependent magnetic interaction, which is a necessary condition for the realization of a Kitaev quantum spin liquid. However, this relativistic electron picture is challenged by an alternate description, in which itinerant electrons are confined to a benzene-like hexagon, keeping the system insulating despite the delocalized nature of the electrons. In this quasi-molecular orbital (QMO) picture, the honeycomb iridates are an unlikely choice for a Kitaev spin liquid. Here we show that the honeycomb iridate Li2IrO3 is best described by a $J_{eff}=1/2$ state at ambient pressure, but crosses over into a QMO state under the application of small (~ 0.1 GPa) hydrostatic pressure. This result illustrates that the physics of iridates is extremely rich due to a delicate balance between electronic bandwidth, spin-orbit coupling, crystal field, and electron correlation.

cond-mat.str-el↗

arXiv2017

Nearest-neighbor Kitaev exchange blocked by charge order in electron doped $α$-RuCl$_{3}$

A quantum spin-liquid might be realized in $α$-RuCl$_{3}$, a honeycomb-lattice magnetic material with substantial spin-orbit coupling. Moreover, $α$-RuCl$_{3}$ is a Mott insulator, which implies the possibility that novel exotic phases occur upon doping. Here, we study the electronic structure of this material when intercalated with potassium by photoemission spectroscopy, electron energy loss spectroscopy, and density functional theory calculations. We obtain a stable stoichiometry at K$_{0.5}$RuCl$_3$. This gives rise to a peculiar charge disproportionation into formally Ru$^{2+}$ (4$d^6$) and Ru$^{3+}$ (4$d^5$). Every Ru 4$d^5$ site with one hole in the $t_{2g}$ shell is surrounded by nearest neighbors of 4$d^6$ character, where the $t_{2g}$ level is full and magnetically inert. Thus, each type of Ru sites forms a triangular lattice and nearest-neighbor interactions of the original honeycomb are blocked.

cond-mat.str-el↗

arXiv2017

Strongly Gapped Spin-Wave Excitation in the Insulating Phase of NaOsO3

NaOsO3 hosts a rare manifestation of a metal-insulator transition driven by magnetic correlations, placing the magnetic exchange interactions in a central role. We use resonant inelastic x-ray scattering to directly probe these magnetic exchange interactions. A dispersive and strongly gapped (58 meV) excitation is observed indicating appreciable spin-orbit coupling in this 5d3 system. The excitation is well described within a minimal model Hamiltonian with strong anisotropy and Heisenberg exchange (J1=J2=13.9 meV). The observed behavior places NaOsO3 on the boundary between localized and itinerant magnetism.

cond-mat.str-el↗

arXiv2017

Anomalous diamagnetic response in multi-band superconductors with time-reversal broken symmetry

Within a Ginzburg-Landau formalism we establish analytically the necessary and sufficient conditions to realize a doubly degenerate superconducting ground state with broken time-reversal symmetry (BTRS) in a multi-band superconductor. Using these results we analyze the ground state of a three-band superconductor in the cylindrical geometry in an external magnetic field. We show that depending on the interband coupling constants, a magnetic flux can induce current density jumps in such superconducting geometries that are related to adiabatic or non-adiabatic transitions from BTRS to time-reversal symmetric states and vice versa. This unusual current induced magnetic flux response can in principle be used experimentally to detect superconducting BTRS ground states as well as corresponding metastable excited states.

cond-mat.supr-con↗

arXiv2017

Doping Dependence of Collective Spin and Orbital Excitations in Spin 1 Quantum Antiferromagnet La$_{2-x}$Sr$_x$NiO$_4$ Observed by X-rays

We report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to \emph{collective} magnetic excitations in $S=1$ systems by probing the Ni $L_3$-edge of La$_{2-x}$Sr$_x$NiO$_4$ ($x = 0, 0.33, 0.45$). The magnetic excitation peak is asymmetric, indicating the presence of single and multi spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. This work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultra-fast pump-probe experiments.

cond-mat.str-el↗

arXiv2016

Experimental realization of type-II Weyl state in non-centrosymmetric TaIrTe$_4$

Recent breakthrough in search for the analogs of fundamental particles in condensed matter systems lead to experimental realizations of 3D Dirac and Weyl semimetals. Weyl state can be hosted either by non-centrosymmetric or magnetic materials and can be of the first or the second type. Several non-centrosymmetric materials have been proposed to be type-II Weyl semimetals, but in all of them the Fermi arcs between projections of multiple Weyl points either have not been observed directly or they were hardly distinguishable from the trivial surface states which significantly hinders the practical application of these materials. Here we present experimental evidence for type-II non-centrosymmetric Weyl state in TaIrTe$_4$ where it has been predicted theoretically. We find direct correspondence between ARPES spectra and calculated electronic structure both in the bulk and the surface and clearly observe the exotic surface states which support the quasi-1D Fermi arcs connecting only four Weyl points. Remarkably, these electronic states are spin-polarized in the direction along the arcs, thus highlighting TaIrTe$_4$ as a novel material with promising application potential.

cond-mat.mes-hall↗

arXiv2016

J$_{eff}$ description of the honeycomb Mott insulator $α$-RuCl$_3$

Novel ground states might be realized in honeycomb lattices with strong spin-orbit coupling. Here we study the electronic structure of $α$-RuCl$_3$, in which the Ru ions are in a d5 configuration and form a honeycomb lattice, by angle-resolved photoemission, x-ray photoemission and electron energy loss spectroscopy supported by density functional theory and multiplet calculations. We find that $α$-RuCl$_3$ is a Mott insulator with significant spin-orbit coupling, whose low energy electronic structure is naturally mapped onto Jeff states. This makes $α$-RuCl$_3$ a promising candidate for the realization of Kitaev physics. Relevant electronic parameters such as the Hubbard energy U, the crystal field splitting 10Dq and the charge transfer energy are evaluated. Furthermore, we observe significant Cl photodesorption with time, which must be taken into account when interpreting photoemission and other surface sensitive experiments.

cond-mat.str-el↗

arXiv2016

Ba2YIrO6: A cubic double perovskite material with Ir5+ ions

Materials with a 5d4 electronic configuration are generally considered to have a nonmagnetic ground state (J=0). Interestingly, Sr2YIrO6 (Ir5+ having 5d4 electronic configuration) was recently reported to exhibit long-range magnetic order at low temperature and the distorted IrO6 octahedra were discussed to cause the magnetism in this material. Hence, a comparison of structurally distorted Sr2YIrO6 with cubic Ba2YIrO6 may shed light on the source of magnetism in such Ir5+ materials with 5d4 configuration. Besides, Ir5+ materials having 5d4 are also interesting in the context of recently predicted excitonic types of magnetism. Here we report a single-crystal-based analysis of the structural, magnetic, and thermodynamic properties of Ba2YIrO6. We observe that in Ba2YIrO6 for temperatures down to 0.4 K, long-range magnetic order is absent but at the same time correlated magnetic moments are present. We show that these moments are absent in fully relativistic ab initio band-structure calculations; hence, their origin is presently unclear.

cond-mat.str-el↗

arXiv2015

Emergent excitation at the magnetic metal-insulator transition in the pyrochlore osmate Cd2Os2O7

The rich physics manifested by 5d oxides falls outside the Mott-Hubbard paradigm used to successfully explain the electronic and magnetic properties of 3d oxides. Much consideration has been given to the extent to which strong spin-orbit coupling (SOC), in the limit of increased bandwidth and reduced electron correlation, drives the formation of novel electronic states, as manifested through the existence of metal-insulator transitions (MITs). SOC is believed to play a dominant role in 5d5 systems such as iridates (Ir4+), undergoing MITs which may or may not be intimately connected to magnetic order, with pyrochlore and perovksite systems being examples of the former and latter, respectively. However, the role of SOC for other 5d configurations is less clear. For example, 5d3 (e.g Os5+) systems are expected to have an orbital singlet and consequently a reduced effect of SOC in the groundstate. The pyrochlore osmate Cd2Os2O7 nonetheless exhibits a MIT intimately entwined with magnetic order with phenomena similar to pyrochlore iridates. Here we report the first resonant inelastic X-ray scattering (RIXS) measurements on an osmium compound, allowing us to determine the salient electronic and magnetic energy scales controlling the MIT in Cd2Os2O7, which we benchmark against detailed quantum chemistry calculations. In particular, we reveal the emergence at the MIT of a magnetic excitation corresponding to a superposition of multiple spin-flip processes from an Ising-like all-in/all-out magnetic groundstate. We discuss our results with respect to the role of SOC in magnetically mediated MITs in 5d systems

cond-mat.str-el↗

arXiv2014

Excitonic quasiparticles in a spin-orbit Mott insulator

In condensed matter systems, out of a large number of interacting degrees of freedom emerge weakly coupled particles, in terms of which most physical properties are described. For example, Landau quasiparticles (QP) determine all electronic properties of a normal metal. The lack of identification of such QPs is major barrier for understanding myriad exotic properties of correlated electrons, such as unconventional superconductivity and non-Fermi liquid behaviours. Here, we report the observation of a composite particle in a Mott insulator Sr2IrO4---and exciton dressed with magnons---that propagates with the canonical characteristics of a QP: a finite QP residue and a lifetime longer than the hopping time scale. The dynamics of this charge-neutral bosonic excitation mirrors the fundamental process of the analogous one-hole propagation in the background of ordered spins, for which a well-defined QP has never been observed. The much narrower linewidth of the exciton reveals the same intrinsic dynamics that is obscured for the hole and is intimately related to the mechanism of high temperature superconductivity.

cond-mat.str-el↗