arXiv subjects

Radu Coldea

Publications and source records attributed to Radu Coldea.

At least 19 recordsLinked to original sources

arXiv2025

From continuum excitations to sharp magnons via transverse magnetic field in the spin-1/2 Ising-like triangular lattice antiferromagnet Na2BaCo(PO4)2

We report high-resolution inelastic neutron scattering measurements of the excitation spectrum in large single crystals of the spin-1/2 triangular lattice Ising-like antiferromagnet Na2BaCo(PO4)2 in magnetic fields applied transverse to the Ising axis. In the high-field polarized phase above a critical field $B_{C}$ we observe sharp magnons, as expected in the case of no exchange disorder. Through simultaneous fits to the dispersions including data in polarizing field along the Ising axis, we obtain an excellent match to an Ising-like XXZ Hamiltonian and rule out previously proposed Kitaev exchanges. In the intermediate-field phase below $B_{C}$, we observe three dispersive modes, out of which only the lowest energy one is sharp and the others are broad and overlap with continuum scattering. We propose that the broadening effects are due to magnon decays into two-magnon excitations and confirm that such processes are kinematically allowed. The continuum scattering becomes progressively stronger upon lowering field and, at 0.25 T and zero field, it dominates the complete spectrum with no clear evidence for even broadened magnon modes. We discuss the relevance of the continuous manifold of mean-field degenerate ground states of the refined Hamiltonian for capturing the observed spectrum in zero field, and compare the data with the one- and two-magnon spectrum averaged over this manifold. We also propose a model of the interlayer couplings to explain the observed finite interlayer magnetic propagation vector of the zero-field magnetic order; this requires the breaking of the mirror symmetry in the nominal P-3m1 space group and through refinement of x-ray diffraction data on an untwinned single crystal, we indeed confirm a rotation of the CoO6 octahedra around the c-axis, which lowers the symmetry to P-3.

cond-mat.str-el↗

arXiv2024

Origin of the insulating state in the Kitaev candidate Cu$_2$IrO$_3$

Through a combination of crystal symmetry analysis and density functional theory calculations we unveil a possible microscopic origin of the unexpected insulating behavior reported in the honeycomb Kitaev material Cu$_2$IrO$_3$. Our study suggests that this material hosts an instability towards charge ordering of the Ir ions, with alternating magnetic Ir$^{4+}$ and non-magnetic Ir$^{3+}$ ions arranged on the honeycomb lattice. In this case, the next-nearest-neighbor interactions that couple magnetic Ir$^{4+}$ ions form an enlarged triangular lattice, instead of the expected honeycomb lattice. The magnetic Cu$^{2+}$ ions located at the centre of the iridium honeycomb voids also form a triangular lattice, and additionally contribute to the magnetization of the system. Together, the interpenetrated Ir$^{4+}$ and Cu$^{2+}$ triangular lattices present a novel type of honeycomb Kitaev lattice composed of two types of magnetic ions.

cond-mat.str-el↗

arXiv2024

Compass-model physics on the hyperhoneycomb lattice in the extreme spin-orbit regime

The physics of spin-orbit entangled magnetic moments of $4d$ and $5d$ transition metal ions on a honeycomb lattice has been much explored in search for unconventional magnetic orders or quantum spin liquids expected for compass spin models, where different bonds in the lattice favour different orientations for the magnetic moments. Realizing such physics with rare-earth ions is a promising route to achieve exotic ground states in the extreme spin orbit limit, however this regime has remained experimentally largely unexplored due to major challenges in materials synthesis. Here we report successful synthesis of powders and single crystals of $\beta$-Na$_2$PrO$_3$, with $4f^{1}$ Pr$^{4+}$ $j_\mathrm{eff}\!=\!1/2$ magnetic moments arranged on a hyperhoneycomb lattice with the same threefold coordination as the planar honeycomb. We find a strongly noncollinear magnetic order with highly dispersive gapped excitations that we argue arise from frustration between bond-dependent, anisotropic off-diagonal exchanges, a compass quantum spin model not explored experimentally so far. Our results show that rare-earth ions on threefold coordinated lattices offer a platform for the exploration of quantum compass spin models in the extreme spin orbit regime, with qualitatively distinct physics from that of $4d$ and $5d$ Kitaev materials.

cond-mat.str-el↗

arXiv2024

Selective synthesis and crystal chemistry of candidate rare earth Kitaev materials: honeycomb and hyperhoneycomb Na$_2$PrO$_3$

Rare earth oxides have attracted interest as a platform for studying frustrated magnetism arising from bond dependent anisotropic interactions. Ordered rock salt compounds Na$_2$PrO$_3$ crystallize in two polymorphs ($\alpha$ and $\beta$) comprising honeycomb and hyperhoneycomb lattices of octahedrally coordinated Pr$^{4+}$ (4$f^1$). Although possible realization of antiferromagnetic Kitaev interactions is anticipated for these phases on the basis of ab initio models, the air-sensitivity of the two polymorphs has hampered reliable crystal growth and physical property measurements. Here, we have succeeded in preparing powder and single crystals of both $\alpha$- and $\beta$-Na$_2$PrO$_3$ using modified synthetic procedures. Revised crystal structures for both polymorphs are obtained from refinement of untwinned single-crystal X-ray diffraction data.

cond-mat.str-el↗

arXiv2024

Anisotropic magnetic interactions in a candidate Kitaev spin liquid close to a metal-insulator transition

In the Kitaev honeycomb model, spins coupled by strongly-frustrated anisotropic interactions do not order at low temperature but instead form a quantum spin liquid with spin fractionalization into Majorana fermions and static fluxes. The realization of such a model in crystalline materials could lead to major breakthroughs in understanding entangled quantum states, however achieving this in practice is a very challenging task. The recently synthesized honeycomb material RuI$_3$ shows no long-range magnetic order down to the lowest probed temperatures and has been theoretically proposed as a quantum spin liquid candidate material on the verge of an insulator to metal transition. Here we report a comprehensive study of the magnetic anisotropy in un-twinned single crystals via torque magnetometry and detect clear signatures of strongly anisotropic and frustrated magnetic interactions. We attribute the development of sawtooth and six-fold torque signal to strongly anisotropic, bond-dependent magnetic interactions by comparing to theoretical calculations. As a function of magnetic field strength at low temperatures, torque shows an unusual non-parabolic dependence suggestive of a proximity to a field-induced transition. Thus, RuI$_3$, without signatures of long-range magnetic order, displays key hallmarks of an exciting new candidate for extended Kitaev magnetism with enhanced quantum fluctuations.

cond-mat.str-el↗

arXiv2024

Anisotropy of the zigzag order in the Kitaev honeycomb magnet $\alpha$-RuBr$_3$

Kitaev materials often order magnetically at low temperatures due to the presence of non-Kitaev interactions. Torque magnetometry is a very sensitive technique for probing the magnetic anisotropy, which is critical in understanding the magnetic ground state. In this work, we report detailed single-crystal torque measurements in the proposed Kitaev candidate honeycomb magnet $\alpha$-RuBr$_3$, which displays zigzag order below 34 K. Based on angular-dependent torque studies in magnetic fields up to 16 T rotated in the plane normal to the honeycomb layers, we find an easy-plane anisotropy with a temperature dependence of the torque amplitude following closely the behaviour of the powder magnetic susceptibility. The torque for field rotated in the honeycomb plane has a clear six-fold periodicity with a saw-tooth shape, reflecting the three-fold symmetry of the crystal structure and stabilization of different zigzag domains depending on the field orientation, with a torque amplitude that follows an order parameter form inside the zigzag phase. By comparing experimental data with theoretical calculations we identify the relevant anisotropic interactions and the role of the competition between different zigzag domains in this candidate Kitaev material.

cond-mat.str-el↗

arXiv2023

Tuning the confinement potential between spinons in the Ising chain CoNb2O6 using longitudinal fields and quantitative determination of the microscopic Hamiltonian

The Ising chain realizes the fundamental paradigm of spin fractionalization, where locally flipping a spin creates two domain walls (spinons) that can separate apart at no energy cost. In a quasi-one-dimensional system, the mean-field effects of the weak three-dimensional couplings confine the spinons into a Zeeman ladder of two-spinon bound states. Here, we experimentally tune the confinement potential between spinons in the quasi-one-dimensional Ising ferromagnet CoNb2O6 by means of an applied magnetic field with a large component along the Ising direction. Using high-resolution single crystal inelastic neutron scattering, we directly observe how the spectrum evolves from the limit of very weak confinement at low field (with many closely-spaced bound states with energies scaling as the field strength to the power 2/3) to very strong confinement at high field (where it consists of a magnon and a dispersive two-magnon bound state, with a linear field dependence). At intermediate fields, we explore how the higher-order bound states disappear from the spectrum as they move to higher energies and overlap with the two-particle continuum. By performing a global fit to the observed spectrum in zero field and high field applied along two orthogonal directions, combined with a quantitative parameterization of the interchain couplings, we propose a refined single chain and interchain Hamiltonian that quantitatively reproduces all observed dispersions and their field dependence.

cond-mat.str-el↗

arXiv2023

Excitations of quantum Ising chain CoNb2O6 in low transverse field: quantitative description of bound states stabilized by off-diagonal exchange and applied field

We present experimental and theoretical evidence of novel bound state formation in the low transverse field ordered phase of the quasi-one-dimensional Ising-like material CoNb$_2$O$_6$. High resolution single crystal inelastic neutron scattering measurements observe that small transverse fields lead to a breakup of the spectrum into three parts, each evolving very differently upon increasing field. This can be naturally understood starting from the excitations of the ordered phase of the transverse field Ising model, domain wall quasiparticles (solitons). Here, the transverse field and a staggered off-diagonal exchange create one-soliton hopping terms with opposite signs. We show that this leads to a rich spectrum and a special field, when the strengths of the off-diagonal exchange and transverse field match, at which solitons become localized; the highest field investigated is very close to this special regime. We solve this case analytically and find three two-soliton continua, along with three novel bound states. Perturbing away from this novel localized limit, we find very good qualitative agreement with the experimental data. We also present calculations using exact diagonalization of a recently refined Hamiltonian model for CoNb$_2$O$_6$ and using diagonalization of the two-soliton subspace, both of which provide a quantitative agreement with the observed spectrum. The theoretical models qualitatively and quantitatively capture a variety of non-trivial features in the observed spectrum, providing insight into the underlying physics of bound state formation.

cond-mat.str-el↗

arXiv2021

Studies on Novel Yb-based Candidate Triangular Quantum Antiferromagnets: Ba3YbB3O9 and Ba3YbB9O18

Yb-based triangular magnets have recently attracted attention as promising candidates to explore frustrated quantum magnetism. However, some candidates have turned out to have significant amounts of site disorder, which significantly affects the low-temperature magnetic behavior. To overcome this issue, Yb-based frustrated systems without structural disorder are required. In this paper, we report physical properties of two Yb-based triangular magnets Ba3YbB3O9 and Ba3YbB9O18, without structural disorder. Via magnetic susceptibility, magnetization, and muon spin rotation measurements, we verified that both Ba3YbB3O9 and, particularly studied for the first time, Ba3YbB9O18 do not show long range magnetic order or glass-like spin freezing down to 0.28 K, but show typical paramagnetic behavior.

cond-mat.str-el↗

arXiv2020

Quantifying and controlling entanglement in the quantum magnet Cs$_2$CoCl$_4$

The lack of methods to experimentally detect and quantify entanglement in quantum matter impedes our ability to identify materials hosting highly entangled phases, such as quantum spin liquids. We thus investigate the feasibility of using inelastic neutron scattering (INS) to implement a model-independent measurement protocol for entanglement based on three entanglement witnesses: one-tangle, two-tangle, and quantum Fisher information (QFI). We perform high-resolution INS measurements on Cs$_2$CoCl$_4$, a close realization of the $S=1/2$ transverse-field XXZ spin chain, where we can control entanglement using the magnetic field, and compare with density-matrix renormalization group calculations for validation. The three witnesses allow us to infer entanglement properties and make deductions about the quantum state in the material. We find QFI to be a particularly robust experimental probe of entanglement, whereas the one- and two-tangles require more careful analysis. Our results lay the foundation for a general entanglement detection protocol for quantum spin systems.

cond-mat.str-el↗

arXiv2020

Avoided quasiparticle decay and enhanced excitation continuum in the spin-1/2 near-Heisenberg triangular antiferromagnet Ba3CoSb2O9

We explore the magnetic excitations of the spin-1/2 triangular antiferromagnet Ba3CoSb2O9 in its 120 degree ordered phase using single-crystal high-resolution inelastic neutron scattering. Sharp magnons with no decay are observed throughout reciprocal space, with a strongly renormalized dispersion and multiple soft modes compared to linear spin wave theory. We propose an empirical parametrization that can quantitatively capture the complete dispersions in the three-dimensional Brillouin zone and explicitly show that the dispersion renormalizations have the direct consequence that one to two magnon decays are avoided throughout reciprocal space, whereas such decays would be allowed for the unrenormalized dispersions. At higher energies, we observe a very strong continuum of excitations with highly-structured intensity modulations extending up at least 4x the maximum one-magnon energy. The one-magnon intensities decrease much faster upon increasing energy than predicted by linear spin wave theory and the higher-energy continuum contains much more intensity than can be accounted for by a two-magnon cross-section, suggesting a significant transfer of spectral weight from the high-energy magnons into the higher-energy continuum states. We attribute the strong dispersion renormalizations and substantial transfer of spectral weight to continuum states to the effect of quantum fluctuations and interactions beyond the spin wave approximation, and make connections to theoretical approaches that might capture such effects. Finally, through measurements in a strong applied magnetic field, we find evidence for magnetic domains with opposite senses for the spin rotation in the 120 degree ordered ground state, as expected in the absence of Dzyaloshinskii-Moriya interactions, when the sense of spin rotation is selected via spontaneous symmetry breaking.

cond-mat.str-el↗

arXiv2020

Glide symmetry breaking and Ising criticality in the quasi-1D magnet CoNb$_2$O$_6$

We construct a microscopic spin-exchange Hamiltonian for the quasi-1D Ising magnet CoNb$_2$O$_6$ that captures detailed and hitherto-unexplained aspects of its dynamic spin structure factor. We perform a symmetry analysis that recalls that an individual Ising chain in this material is buckled, with two sites in each unit cell related by a glide symmetry. Combining this with numerical simulations benchmarked against neutron scattering experiments, we argue that the single-chain Hamiltonian contains a staggered spin-exchange term. We further argue that the transverse-field-tuned quantum critical point in CoNb$_2$O$_6$ corresponds to breaking this glide symmetry, rather than an on-site Ising symmetry as previously believed. This gives a unified microscopic explanation of the dispersion of confined states in the ordered phase and `quasiparticle breakdown' in the polarized phase at high transverse field.

cond-mat.str-el↗

arXiv2018

Spin dynamics of coupled spin ladders near quantum criticality in Ba2CuTeO6

We report inelastic neutron scattering measurements of the magnetic excitations in Ba2CuTeO6, proposed by ab initio calculations to magnetically realize weakly coupled antiferromagnetic two-leg spin-1/2 ladders. Isolated ladders are expected to have a singlet ground state protected by a spin gap. Ba2CuTeO6 orders magnetically, but with a small Neel temperature relative to the exchange strength, suggesting that the interladder couplings are relatively small and only just able to stabilize magnetic order, placing Ba2CuTeO6 close in parameter space to the critical point separating the gapped phase and Neel order. Through comparison of the observed spin dynamics with linear spin wave theory and quantum Monte Carlo calculations, we propose values for all relevant intra- and interladder exchange parameters, which place the system on the ordered side of the phase diagram in proximity to the critical point. We also compare high field magnetization data with quantum Monte Carlo predictions for the proposed model of coupled ladders.

cond-mat.str-el↗

arXiv2017

Probing $\alpha$-RuCl$_3$ Beyond Magnetic Order: Effects of Temperature and Magnetic Field

Recent studies have brought $\alpha$-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 $\alpha$-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 semi-classical 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 roadmap for further studies of these regimes.

cond-mat.str-el↗

arXiv2016

Spin dynamics of counterrotating Kitaev spirals via duality

Incommensurate spiral order is a common occurrence in frustrated magnetic insulators. Typically, all magnetic moments rotate uniformly, through the same wavevector. However the honeycomb iridates family Li2IrO3 shows an incommensurate order where spirals on neighboring sublattices are counter-rotating, giving each moment a different local environment. Theoretically describing its spin dynamics has remained a challenge: the Kitaev interactions proposed to stabilize this state, which arise from strong spin-orbit effects, induce magnon umklapp scattering processes in spin-wave theory. Here we propose an approach via a (Klein) duality transformation into a conventional spiral of a frustrated Heisenberg model, allowing a direct derivation of the dynamical structure factor. We analyze both Kitaev and Dzyaloshinskii-Moriya based models, both of which can stabilize counterrotating spirals, but with different spin dynamics, and we propose experimental tests to identify the origin of counterrotation.

cond-mat.str-el↗

arXiv2014

Unified theory of spiral magnetism in the harmonic-honeycomb iridates {\alpha}, {\beta}, {\gamma} Li2IrO3

A family of insulating iridates with chemical formula Li$_2$IrO$_3$ has recently been discovered, featuring three distinct crystal structures $\alpha,\beta,\gamma$ (honeycomb, hyperhoneycomb, stripyhoneycomb). Measurements on the three-dimensional polytypes, $\beta$- and $\gamma$-Li$_2$IrO$_3$, found that they magnetically order into remarkably similar spiral phases, exhibiting a non-coplanar counter-rotating spiral magnetic order with equivalent q=0.57 wavevectors. We examine magnetic Hamiltonians for this family and show that the same triplet of nearest-neighbor Kitaev-Heisenberg-Ising (KJI) interactions reproduces this spiral order on both $\beta,\gamma$-Li$_2$IrO$_3$ structures. We analyze the origin of this phenomenon by studying the model on a 1D zigzag chain, a structural unit common to the three polytypes. The zigzag-chain solution transparently shows how the Kitaev interaction stabilizes the counter-rotating spiral, which is shown to persist on restoring the inter-chain coupling. Our minimal model makes a concrete prediction for the magnetic order in $\alpha$-Li$_2$IrO$_3$.

cond-mat.str-el↗

arXiv2014

"Quasi-particle breakdown" in the quasi-one-dimensional Ising ferromagnet CoNb$_2$O$_6$

We present experimental and theoretical evidence that an interesting quantum many-body effect -- quasi-particle breakdown -- occurs in the quasi-one-dimensional spin-1/2 Ising-like ferromagnet CoNb$_2$O$_6$ in its paramagnetic phase at high transverse field as a result of explicit breaking of spin inversion symmetry. We propose a quantum spin Hamiltonian capturing the essential one-dimensional physics of CoNb$_2$O$_6$ and determine the exchange parameters of this model by fitting the calculated single particle dispersion to the one observed experimentally in applied transverse magnetic fields. We present high-resolution inelastic neutron scattering measurements of the single particle dispersion which observe "anomalous broadening" effects over a narrow energy range at intermediate energies. We propose that this effect originates from the decay of the one particle mode into two-particle states. This decay arises from (i) a finite overlap between the one-particle dispersion and the two-particle continuum in a narrow energy-momentum range and (ii) a small misalignment of the applied field away from the direction perpendicular to the Ising axis in the experiments, which allows for non-zero matrix elements for decay by breaking the $\mathbb{Z}_2$ spin inversion symmetry of the Hamiltonian.

cond-mat.str-el↗

arXiv2014

A new spin-anisotropic harmonic honeycomb iridate

The physics of Mott insulators underlies diverse phenomena ranging from high temperature superconductivity to exotic magnetism. Although both the electron spin and the structure of the local orbitals play a key role in this physics, in most systems these are connected only indirectly --- via the Pauli exclusion principle and the Coulomb interaction. Iridium-based oxides (iridates) open a further dimension to this problem by introducing strong spin-orbit interactions, such that the Mott physics has a strong orbital character. In the layered honeycomb iridates this is thought to generate highly spin-anisotropic interactions, coupling the spin orientation to a given spatial direction of exchange and leading to strongly frustrated magnetism. The potential for new physics emerging from such interactions has driven much scientific excitement, most recently in the search for a new quantum spin liquid, first discussed by Kitaev \cite{kitaev_anyons_2006}. Here we report a new iridate structure that has the same local connectivity as the layered honeycomb, but in a three-dimensional framework. The temperature dependence of the magnetic susceptibility exhibits a striking reordering of the magnetic anisotropy, giving evidence for highly spin-anisotropic exchange interactions. Furthermore, the basic structural units of this material suggest the possibility of a new family of structures, the `harmonic honeycomb' iridates. This compound thus provides a unique and exciting glimpse into the physics of a new class of strongly spin-orbit coupled Mott insulators.

cond-mat.mtrl-sci↗