# Publications

## Probing α-RuCl_{3} Beyond Magnetic Order: Effects of Temperature and Magnetic Field.

Physical review letters **120** (2018) 077203-

Recent studies have brought α-RuCl_{3} to the forefront of experimental searches for materials realizing Kitaev spin-liquid physics. This material exhibits strongly anisotropic exchange interactions afforded by the spin-orbit coupling of the 4d Ru centers. We investigate the dynamical response at finite temperature and magnetic field for a realistic model of the magnetic interactions in α-RuCl_{3}. These regimes are thought to host unconventional paramagnetic states that emerge from the suppression of magnetic order. Using exact diagonalization calculations of the quantum model complemented by semiclassical analysis, we find a very rich evolution of the spin dynamics as the applied field suppresses the zigzag order and stabilizes a quantum paramagnetic state that is adiabatically connected to the fully polarized state at high fields. At finite temperature, we observe large redistributions of spectral weight that can be attributed to the anisotropic frustration of the model. These results are compared to recent experiments and provide a road map for further studies of these regimes.

## Quasiparticle Breakdown and Spin Hamiltonian of the Frustrated Quantum Pyrochlore Yb_{2}Ti_{2}O_{7} in a Magnetic Field.

Physical review letters **119** (2017) 057203-

The frustrated pyrochlore magnet Yb_{2}Ti_{2}O_{7} has the remarkable property that it orders magnetically but has no propagating magnons over wide regions of the Brillouin zone. Here we use inelastic neutron scattering to follow how the spectrum evolves in cubic-axis magnetic fields. At high fields we observe, in addition to dispersive magnons, a two-magnon continuum, which grows in intensity upon reducing the field and overlaps with the one-magnon states at intermediate fields leading to strong renormalization of the dispersion relations, and magnon decays. Using heat capacity measurements we find that the low- and high-field regions are smoothly connected with no sharp phase transition, with the spin gap increasing monotonically in field. Through fits to an extensive data set of dispersion relations combined with magnetization measurements, we reevaluate the spin Hamiltonian, finding dominant quantum exchange terms, which we propose are responsible for the anomalously strong fluctuations and quasiparticle breakdown effects observed at low fields.

## Topological triplon modes and bound states in a Shastry-Sutherland magnet

NATURE PHYSICS **13** (2017) 736-+

## Magnetic Field Dependence of Excitations Near Spin-Orbital Quantum Criticality.

Physical review letters **118** (2017) 067205-

The spinel FeSc_{2}S_{4} has been proposed to realize a near-critical spin-orbital singlet (SOS) state, where entangled spin and orbital moments fluctuate in a global singlet state on the verge of spin and orbital order. Here we report powder inelastic neutron scattering measurements that observe the full bandwidth of magnetic excitations and we find that spin-orbital triplon excitations of an SOS state can capture well key aspects of the spectrum in both zero and applied magnetic fields up to 8.5 T. The observed shift of low-energy spectral weight to higher energies upon increasing applied field is naturally explained by the entangled spin-orbital character of the magnetic states, a behavior that is in strong contrast to spin-only singlet ground state systems, where the spin gap decreases upon increasing applied field.

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

Scientific reports **6** (2016) 35362-

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. 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 contrast to classical vapor transport, the process is essentially isothermal and a temperature gradient of minor importance. 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. A successful use of this simple and low cost technique for various other materials is anticipated.

## Incommensurate counterrotating magnetic order stabilized by Kitaev interactions in the layered honeycomb alpha-Li2IrO3

PHYSICAL REVIEW B **93** (2016) ARTN 195158

## Spin dynamics of counterrotating Kitaev spirals via duality

PHYSICAL REVIEW B **94** (2016) ARTN 201110

## Monoclinic crystal structure of alpha-RuCl3 and the zigzag antiferromagnetic ground state

PHYSICAL REVIEW B **92** (2015) ARTN 235119

## Unified theory of spiral magnetism in the harmonic-honeycomb iridates alpha, beta, and gamma Li2IrO3

PHYSICAL REVIEW B **91** (2015) ARTN 245134

## Unconventional magnetic order on the hyperhoneycomb Kitaev lattice in beta-Li2IrO3: Full solution via magnetic resonant x-ray diffraction

PHYSICAL REVIEW B **90** (2014) ARTN 205116

## Cascade of field-induced magnetic transitions in a frustrated antiferromagnetic metal

PHYSICAL REVIEW B **90** (2014) ARTN 020401

## Realization of a three-dimensional spin-anisotropic harmonic honeycomb iridate.

Nature communications **5** (2014) 4203-

Spin and orbital quantum numbers play a key role in the physics of Mott insulators, but in most systems they are connected only indirectly--via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) introduce strong spin-orbit coupling directly, such that these numbers become entwined together and the Mott physics attains a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin-anisotropic magnetic interactions, coupling the spin to a given spatial direction of exchange and leading to strongly frustrated magnetism. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb and exhibits striking evidence for highly spin-anisotropic exchange. The basic structural units of this material suggest that a new family of three-dimensional structures could exist, the 'harmonic honeycomb' iridates, of which the present compound is the first example.

## Quasiparticle breakdown in the quasi-one-dimensional Ising ferromagnet CoNb2O6

PHYSICAL REVIEW B **90** (2014) ARTN 174406

## Noncoplanar and counterrotating incommensurate magnetic order stabilized by Kitaev interactions in γ-Li(2)IrO(3).

Physical review letters **113** (2014) 197201-

Materials that realize Kitaev spin models with bond-dependent anisotropic interactions have long been searched for, as the resulting frustration effects are predicted to stabilize novel forms of magnetic order or quantum spin liquids. Here, we explore the magnetism of γ-Li(2)IrO(3), which has the topology of a three-dimensional Kitaev lattice of interconnected Ir honeycombs. Using magnetic resonant x-ray diffraction, we find a complex, yet highly symmetric incommensurate magnetic structure with noncoplanar and counterrotating Ir moments. We propose a minimal Kitaev-Heisenberg Hamiltonian that naturally accounts for all key features of the observed magnetic structure. Our results provide strong evidence that γ-Li(2)IrO(3) realizes a spin Hamiltonian with dominant Kitaev interactions.

## Excitations in the quantum paramagnetic phase of the quasi-one-dimensional Ising magnet CoNb2O6 in a transverse field: Geometric frustration and quantum renormalization effects

PHYSICAL REVIEW B **90** (2014) ARTN 014418

## Spin waves and revised crystal structure of honeycomb iridate Na2IrO3

Physical Review Letters **108** (2012) 127204

We report inelastic neutron scattering measurements on Na2IrO3, a candidate for the Kitaev spin model on the honeycomb lattice. We observe spin-wave excitations below 5 meV with a dispersion that can be accounted for by including substantial further-neighbor exchanges that stabilize zig-zag magnetic order. The onset of long-range magnetic order below 15.3 K is confirmed via the observation of oscillations in zero-field muon-spin rotation experiments. Combining single-crystal diffraction and density functional calculations we propose a revised crystal structure model with significant departures from the ideal 90 deg Ir-O-Ir bonds required for dominant Kitaev exchange.

## Anomalous high-energy spin excitations in the high-Tc superconductor-parent antiferromagnet La₂CuO₄.

Phys Rev Lett **105** (2010) 247001-

Inelastic neutron scattering is used to investigate the collective magnetic excitations of the high-temperature superconductor-parent antiferromagnet La2CuO4. We find that while the lower energy excitations are well described by spin-wave theory, including one- and two-magnon scattering processes, the high-energy spin waves are strongly damped near the (1/2, 0) position in reciprocal space and merge into a momentum dependent continuum. This anomalous damping indicates the decay of spin waves into other excitations, possibly unbound spinon pairs.

## Quantum criticality in an Ising chain: experimental evidence for emergent E8 symmetry.

Science **327** (2010) 177-180

Quantum phase transitions take place between distinct phases of matter at zero temperature. Near the transition point, exotic quantum symmetries can emerge that govern the excitation spectrum of the system. A symmetry described by the E8 Lie group with a spectrum of eight particles was long predicted to appear near the critical point of an Ising chain. We realize this system experimentally by using strong transverse magnetic fields to tune the quasi-one-dimensional Ising ferromagnet CoNb2O6 (cobalt niobate) through its critical point. Spin excitations are observed to change character from pairs of kinks in the ordered phase to spin-flips in the paramagnetic phase. Just below the critical field, the spin dynamics shows a fine structure with two sharp modes at low energies, in a ratio that approaches the golden mean predicted for the first two meson particles of the E8 spectrum. Our results demonstrate the power of symmetry to describe complex quantum behaviors.

## Magnetic order and dynamics of the charge-ordered antiferromagnet La1.5Sr0.5CoO4

Phys Rev B AIP **80** (2009) 134414

We describe neutron-scattering experiments performed to investigate the magnetic order and dynamics of half-doped La1.5Sr0.5CoO4. This layered perovskite exhibits a near-ideal checkerboard pattern of Co2+/Co3+ charge order at temperatures below ~800 K. Magnetic correlations are observed at temperatures below ~60 K but the magnetic order only becomes established at 31 K, a temperature at which a kink is observed in the susceptibility. On warming above 31 K we observed a change in the magnetic correlations which we attribute either to a spin canting or to a change in the proportion of inequivalent magnetic domains. The magnetic excitation spectrum is dominated by an intense band extending above a gap of approximately 3 meV up to a maximum energy of 16 meV. A weaker band exists in the energy range of 20–30 meV. We show that the excitation spectrum is in excellent quantitative agreement with the predictions of a spin-wave theory generalized to include the full magnetic degrees of freedom of high-spin Co2+ ions in an axially distorted crystal field, coupled by Heisenberg exchange interactions. The magnetic order is found to be stabilized by dominant antiferromagnetic Co2+–Co2+ interactions acting in a straight line through Co3+. No evidence is found for magnetic scattering from the Co3+ ions, supporting the view that Co3+ is in the S=0 state in this material.

## Spin wave dynamics of 2d and 3d heisenberg antiferromagnets

Acta Physica Polonica A **115** (2009) 19-24

The excitations of the 2D Heisenberg antiferromagnet, Rb2MnF4, were studied using neutron scattering techniques with the MAPS spectrometer at the ISIS facility of Rutherford Appleton Laboratory. Measurements were made of the magnetic excitations over the whole 2D Brillouin zone at 6 temperatures below the ordering temperature of 38 K and 6 temperatures above. It was found that the excitations were well defined if their wave vectors were larger than the inverse correlation length and were overdamped if the wave vectors of the excitations were smaller than the inverse correlation length. In more detail we have compared our experimental results with the results of classical simulations and the results gave a very adequate description of the experimental results except at the lowest temperature where the form of the dispersion relation was correct but the energies of the excitations were in error. Nevertheless, classical simulations do provide an effcient and easily implemented methodology for modelling the excitations in the Heisenberg magnets. The damping of the excitations was experimentally found to follow a T2behaviour over all wave vector and energy scales. This is in agreement with the classical simulations but inconsistent with analytic theories of the damping for the 2D Heisenberg model and in particular does not agree with hydrodynamic behaviour or dynamic scaling. The result is similar to that found in 3D Heisenberg systems and suggests that more analytic theory is needed to explain the experimental results for both 2D and 3D Heisenberg magnets.