arXiv subjects

Barry Winn

Publications and source records attributed to Barry Winn.

At least 19 recordsLinked to original sources

arXiv2026

Chiral Magnon Mixing by Symmetry-Breaking in Collinear Ferrimagnets

Magnons in ferromagnets possess spin angular momentum defined by right-handed precession of the moment around the magnetization direction. In antiferromagnets with no net magnetization, left-and right-handed magnons are degenerate in the absence of an applied field. Ferrimagnets possess uncompensated magnetic sublattices, which should natively possess right-and left-handed magnons where their energy is split by the internal molecular field. Here, we show that RMn6Sn6 (R = Tb, Er) ferrimagnets possess right and left-handed magnon bands that cross at finite momentum (k) within the basal plane, defining modes with opposite dynamical chirality. Depending on the symmetry of the ferrimagnetic order, which may be manipulated by varying the rare-earth magnetic anisotropy or with applied field, the band crossing may remain a nodal line or may be gapped. The gapped modes contain hybridized chiral excitations whose chirality becomes k-dependent.

cond-mat.str-el↗

arXiv2024

Phase Diagram and Spectroscopic Signatures of a Supersolid in Quantum Ising Magnet K$_2$Co(SeO$_3$)$_2$

A supersolid is a quantum-entangled state of matter exhibiting the dual characteristics of superfluidity and solidity. Theory predicts that hard-core bosons with repulsive interactions on a triangular lattice can form supersolid phases at half filling and near complete filling. Leveraging an exact mapping between bosons and spin-$\frac{1}{2}$ degrees of freedom, we investigate these phases in the spin-$\frac{1}{2}$ triangular-lattice antiferromagnet \K212 with exchange constants $J_z = 2.96(2)$~meV and $J_{\perp} = 0.21(3)$~meV. At zero field, neutron diffraction reveals the gradual development for $T<15$~K of quasi-two-dimensional $\sqrt{3}\times\sqrt{3}$ magnetic order with $Z_3$ translational symmetry breaking (solidity) albeit with 44(5)% reduced amplitude at $T=0.3$~K indicating strong quantum fluctuations. These are apparent in equidistant bands of continuum neutron scattering for $\hslash\omega_n\approx n\times J_z$, where $n=0,1,2,3$. The lowest energy ($n=0$) $\bf Q$-dependent continuum has a lower resonant edge and includes a quasi-elastic component at K $(\frac{1}{3}\frac{1}{3})$ consistent with broken $U(1)$ spin rotational symmetry (boson superfluidity). Competing instabilities are apparent in soft albeit finite-energy modes at M $(\frac{1}{2}0)$ and at $\frac{1}{2}$K $(\frac{1}{6}\frac{1}{6})$. For $\bf c$-axis-oriented magnetic fields $17~{\rm T} <\mu_0 H< 21~{\rm T}$ that almost saturate the magnetization, corresponding to nearly filling the lattice with bosons, we find a new phase consistent with a second supersolid. These phases are separated by a pronounced 1/3 magnetization plateau that supports coherent spin waves, from which we determine the spin Hamiltonian.

cond-mat.str-el↗

arXiv2024

Continuum of magnetic excitations in the Kitaev honeycomb iridate D$_3$LiIr$_2$O$_6$

Inelastic neutron scattering (INS) measurements of powder D$_3(^{7}$Li)($^{193}$Ir)$_2$O$_6$ reveal low energy magnetic excitations with a scattering cross section that is broad in $|Q|$ and consistent with a Kitaev spin-liquid (KSL) state. The magnetic nature of the excitation spectrum is demonstrated by longitudinally polarized neutron studies. The total magnetic moment of 1.7(2)$\mu_B$/Ir inferred from the total magnetic scattering cross section is consistent with the effective moment inferred from magnetic susceptibility data and expectations for the $J_{\rm eff}=1/2$ single ion state. The rise in the dynamic correlation function ${\cal S}(Q,\omega)$ for $\hbar\omega<5~$meV can be described by a nearest-neighbor Kitaev model with interaction strength $K\approx-13(5)$~meV. Exchange disorder associated with the mixed D-Li site could play an important role in stabilizing the low $T$ quantum fluctuating state.

cond-mat.str-el↗

arXiv2023

Implementation of a laser-neutron pump-probe capability at HYSPEC

Exciting new fundamental scientific questions are currently being raised regarding nonequilibrium dynamics in spin systems, as this directly relates to low power and low loss energy transport for spintronics. Inelastic neutron scattering (INS) is an indispensable tool to study spin excitations in complex magnetic materials. However, conventional INS spectrometers currently only perform steady-state measurements and probe averaged properties over many collision events between spin excitations in thermodynamic equilibrium, while the exact picture of re-equilibration of these excitations remains unknown. In this work, we designed and implemented a time-resolved laser-neutron pump-probe capability at HYSPEC (Hybrid Spectrometer, beamline 14-B) at the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory. This capability allows us to excite out-of-equilibrium magnons with a nanosecond pulsed laser source and probe the resulting dynamics using INS. Here, we discussed technical aspects to implement such a capability in a neutron beamline, including choices of suitable neutron instrumentation and material systems, laser excitation scheme, experimental configurations, and relevant firmware and software development to allow for time-synchronized pump-probe measurements. We demonstrated that the laser-induced nonequilibrium structural factor is able to be resolved by INS in a quantum magnet. The method developed in this work will provide SNS with advanced capabilities for performing out-of-equilibrium measurements, opening up an entirely new research direction to study out-of-equilibrium phenomena using neutrons.

cond-mat.mtrl-sci↗

arXiv2023

Coexistence of symmetry-protected topological order and Neel order in the spin-1/2 ladder antiferromagnet C9H18N2CuBr4

Topological phases of matter are beyond the paradigm of Landau's symmetry breaking and have challenged our understanding of condensed matter systems. Here we report a new type of symmetry-protected topological phase of matter in the spin-1/2 coupled two-leg ladder antiferromagnet C9H18N2CuBr4, DLCB for short. In this two-sublattice antiferromagnet with a weak easy-axis anisotropy, we find no evidence of a conventional spin-flop transition in the magnetization with the magnetic field applied parallel to the easy axis at T=0.4 K, well below TN=2.0 K. Moreover, the temperature dependence of the gapped transverse excitations across TN indicates that they are not the conventional S=1 magnons associated with explicit symmetry breaking. Instead, the thermal renormalization of the gap energy shows a remarkable agreement with a calculation for the three-dimensional O(3) nonlinear sigma model. Accordingly, the spin gap in DLCB is not due to the spin anisotropy but to the separation between a spin singlet state and a triplet excited state. Since an antiferromagnetic spin-1/2 ladder systems can be mapped onto the spin-1 chain, the notion of the Haldane gap is proposed to explain the opening of the spin gap in DLCB. Therefore, the ground state of DLCB is best described as a quantum superposition of a Haldane phase and a Neel-ordered phase, which resembles the quantum state of a qubit in quantum computing. Our results indicate the presence of a symmetry-protected topological order coexisting with an antiferromagnetic order in this material.

cond-mat.str-el↗

arXiv2022

Magnetic Pair Distribution Function Data Using Polarized Neutrons and ad hoc Corrections

We report the first example of magnetic pair distribution function (mPDF) data obtained through use of neutron polarization analysis. Using the antiferromagnetic semiconductor MnTe as a test case, we present high-quality mPDF data collected on the HYSPEC instrument at the Spallation Neutron Source using longitudinal polarization analysis to isolate the magnetic scattering cross section. Clean mPDF patterns are obtained for MnTe in both the magnetically ordered state and the correlated paramagnet state, where only short-range magnetic order is present. We also demonstrate significant improvement in the quality of high-resolution mPDF data through application of ad hoc corrections that require only minimal human input, minimizing potential sources of error in the data processing procedure. We briefly discuss the current limitations and future outlook of mPDF analysis using polarized neutrons. Overall, this work provides a useful benchmark for mPDF analysis using polarized neutrons and provides an encouraging picture of the potential for routine collection of high-quality mPDF data.

cond-mat.mtrl-sci↗

arXiv2022

Geometrical frustration versus Kitaev interactions in BaCo$_2$(AsO$_4$)$_2$

Recently, Co-based honeycomb magnets have been proposed as promising candidate materials to host the Kitaev spin liquid state. One of the front-runners is BaCo$_2$(AsO$_4$)$_2$ (BCAO), where it was suggested that the exchange processes between Co$^{2+}$ ions via the surrounding edge-sharing oxygen octahedra could give rise to bond-dependent Kitaev interactions. In this work, we present and analyze comprehensive inelastic neutron scattering studies of BCAO with fields in the honeycomb plane. Combining the constraints from the magnon excitations in the high-field polarized state and the inelastic spin structure factor measured in zero magnetic field, we examine two leading theoretical models: the Kitaev-type \JKG model and the \XXZ model. We show that the existing experimental data can be consistently accounted for by the \XXZ model but not by the \JKG model, and we discuss the implications of these results for the realization of a spin liquid phase in BCAO and more generally for the realization of the Kitaev model in cobaltates.

cond-mat.str-el↗

arXiv2022

The generalized quasiharmonic approximation via space group irreducible derivatives

The quasiharmonic approximation (QHA) is the simplest nontrivial approximation for interacting phonons under constant pressure, bringing the effects of anharmonicity into temperature dependent observables. Nonetheless, the QHA is often implemented with additional approximations due to the complexity of computing phonons under arbitrary strains, and the generalized QHA, which employs constant stress boundary conditions, has not been completely developed. Here we formulate the generalized QHA, providing a practical algorithm for computing the strain state and other observables as a function of temperature and true stress. We circumvent the complexity of computing phonons under arbitrary strains by employing irreducible second order displacement derivatives of the Born-Oppenheimer potential and their strain dependence, which are efficiently and precisely computed using the lone irreducible derivative approach. We formulate two complementary strain parametrizations: a discretized strain grid interpolation and a Taylor series expansion in symmetrized strain. We illustrate our approach by evaluating the temperature and pressure dependence of the elastic constant tensor and the thermal expansion in thoria (ThO$_2$) using density functional theory with three exchange-correlation functionals. The QHA results are compared to our measurements of the elastic constant tensor using time domain Brillouin scattering and inelastic neutron scattering. Our irreducible derivative approach simplifies the implementation of the generalized QHA, which will facilitate reproducible, data driven applications.

cond-mat.mtrl-sci↗

arXiv2022

Validating First-Principles Phonon Lifetimes via Inelastic Neutron Scattering

Phonon lifetimes are a key component of quasiparticle theories of transport, yet first-principles lifetimes are rarely directly compared to inelastic neutron scattering (INS) results. Existing comparisons show discrepancies even at temperatures where perturbation theory is expected to be reliable. In this work, we demonstrate that the reciprocal space voxel ($q$-voxel), which is the finite region in reciprocal space required in INS data analysis, must be explicitly accounted for within theory in order to draw a meaningful comparison. We demonstrate accurate predictions of peak widths of the scattering function when accounting for the $q$-voxel in CaF$_2$ and ThO$_2$. Passing this test implies high fidelity of the phonon interactions and the approximations used to compute the Green's function, serving as critical benchmark of theory, and indicating that other material properties should be accurately predicted; which we demonstrate for thermal conductivity.

cond-mat.mtrl-sci↗

arXiv2021

Massless Dirac magnons in the two dimensional van der Waals honeycomb magnet CrCl3

Two dimensional van der Waals ferromagnets with honeycomb structures are expected to host the bosonic version of Dirac particles in their magnon excitation spectra. Using inelastic neutron scattering, we study spin wave excitations in polycrystalline CrCl$_3$, which exhibits ferromagnetic honeycomb layers with antiferromagnetic stackings along the $c$-axis. For comparison, polycrystal samples of CrI$_3$ with different grain sizes are also studied. We find that the powder-averaged spin wave spectrum of CrCl$_3$ at $T$ = 2 K can be adequately explained by the two dimensional spin Hamiltonian including in-plane Heisenberg exchanges only. The observed excitation does not exhibit noticeable broadening in energy, which is in remarkable contrast to the substantial broadening observed in CrI$_3$. Based on these results, we conclude that the ferromagnetic phase of CrCl$_3$ hosts massless Dirac magnons and is thus not topological.

cond-mat.str-el↗

arXiv2021

Direct Observation of Chiral Phonons by Inelastic X-ray Scattering

Phonon chirality has attracted intensive attention since it breaks the traditional cognition that phonons are linear propagating bosons. This new quasiparticle property has been extensively studied theoretically and experimentally. However, characterization of the phonon chirality throughout the full Brillouin zone is still not possible due to the lack of available experimental tools. In this work, phonon dispersion and chirality of tungsten carbide were investigated by millielectronvolt energy-resolution inelastic X-ray scattering. The atomistic calculation indicates that in-plane longitudinal and transverse acoustic phonons near K and K$^\prime$ points are circularly polarized due to the broken inversion symmetry. Anomalous inelastic X-ray scattering by these circularly polarized phonons was observed and attributed to their chirality. Our results show that inelastic X-ray scattering can be utilized to characterize phonon chirality in materials and suggest that a revision to the phonon scattering function is necessary.

cond-mat.mtrl-sci↗

arXiv2021

Magnetic field effect on topological spin excitations in CrI$_3$

The search for topological spin excitations in recently discovered two-dimensional (2D) van der Waals (vdW) magnetic materials is important because of their potential applications in dissipation-less spintronics. In the 2D vdW ferromagnetic (FM) honeycomb lattice CrI$_3$(T$_C$= 61 K), acoustic and optical spin waves were found to be separated by a gap at the Dirac points. The presence of such a gap is a signature of topological spin excitations if it arises from the next nearest neighbor(NNN) Dzyaloshinskii-Moriya (DM) or bond-angle dependent Kitaev interactions within the Cr honeycomb lattice. Alternatively, the gap is suggested to arise from an electron correlation effect not associated with topological spin excitations. Here we use inelastic neutron scattering to conclusively demonstrate that the Kitaev interactions and electron correlation effects cannot describe spin waves, Dirac gap and their in-plane magnetic field dependence. Our results support the DM interactions being the microscopic origin of the observed Dirac gap. Moreover, we find that the nearest neighbor (NN) magnetic exchange interactions along the axis are antiferromagnetic (AF)and the NNN interactions are FM. Therefore, our results unveil the origin of the observedcaxisAF order in thin layers of CrI$_3$, firmly determine the microscopic spin interactions in bulk CrI$_3$, and provide a new understanding of topology-driven spin excitations in 2D vdW magnets.

cond-mat.str-el↗

arXiv2021

Neutron Scattering Study of Magnetic Anisotropy in a Tetragonal Antiferromagnet Bi$_2$CuO$_4$

We present a comprehensive study of magnon excitations in the tetragonal easy-plane anti-ferromagnet Bi$_2$CuO$_4$ using inelastic neutron scattering and spin wave analyses. The nature of low energy magnons, and hence the anisotropy in this material, has been controversial. We show unambiguously that the low energy magnon spectrum consists of a gapped and a gapless mode, which we attribute to out-of-plane and in-plane spin fluctuations, respectively. We modelled the observed magnon spectrum using linear spin wave analysis of a minimal anisotropic spin model motivated by the lattice symmetry. By studying the magnetic field dependence of the (1, 0, 0) Bragg peak intensity and the in-plane magnon intensity, we observed a spin-flop transition in the $ab$ plane at $\sim0.4$~T which directly indicates the existence of a small in-plane anisotropy that is classically forbidden. It is only by taking into account magnon zero-point fluctuations beyond the linear spin wave approximation, we could explain this in-plane anisotropy and its magnitude, the latter of which is deduced from critical field of the spin-flop transition. The microscopic origins of the observed anisotropic interactions are also discussed. We found that our data is inconsistent with a large Dzyaloshinskii-Moriya interaction, which suggests a potential departure of Bi$_2$CuO$_4$ from the conventional theories of magnetic anisotropy for other cuprates.

cond-mat.str-el↗

arXiv2020

Spin dynamics and a nearly continuous magnetic phase transition in an entropy-stabilized oxide antiferromagnet

The magnetic order and the spin dynamics in the antiferromagnetic entropy-stabilized oxide (Mg$_{0.2}$Co$_{0.2}$Ni$_{0.2}$Cu$_{0.2}$Zn$_{0.2}$)O (MgO-ESO) have been studied using muon spin relaxation ($μ$SR) and inelastic neutron scattering. We find that antiferromagnetic order develops gradually in the sample volume as it is cooled below 140 K, becoming fully ordered around 100 K. The spin dynamics show a critical slowing down in the vicinity of the transition, and the magnetic order parameter grows continuously in the ordered state. These results indicate that the antiferromagnetic transition is continuous but proceeds with a Gaussian distribution of ordering temperatures. The magnetic contribution to the specific heat determined from inelastic neutron scattering likewise shows a broad feature centered around 120 K. High-resolution inelastic neutron scattering further reveals an initially gapped spectrum at low temperature which sees an increase in a quasielastic contribution upon heating until the ordering temperature.

cond-mat.mtrl-sci↗

arXiv2019

Neutron scattering signatures of a quantum spin ice

Quantum spin ice is an appealing proposal of a quantum spin liquid - systems where the magnetic moments of the constituent electron spins evade classical long-range order to form an exotic state that is quantum entangled and coherent over macroscopic length scales. Such phases are at the edge of our current knowledge in condensed matter as they go beyond the established paradigm of symmetry-breaking order and associated excitations. Neutron scattering experiments on the pyrochlore material Pr$_2$Hf$_2$O$_7$ reveal signatures of a quantum spin ice state that were predicted by theory.

cond-mat.str-el↗

arXiv2019

Experimental signatures of emergent quantum electrodynamics in Pr$_2$Hf$_2$O$_7$

In a quantum spin liquid, the magnetic moments of the constituent electron spins evade classical long-range order to form an exotic state that is quantum entangled and coherent over macroscopic length scales [1-2]. Such phases offer promising perspectives for device applications in quantum information technologies, and their study can reveal fundamentally novel physics in quantum matter. Quantum spin ice is an appealing proposal of one such state, in which the fundamental ground state properties and excitations are described by an emergent U(1) lattice gauge theory [3-7]. This quantum-coherent regime has quasiparticles that are predicted to behave like magnetic and electric monopoles, along with a gauge boson playing the role of an artificial photon. However, this emergent lattice quantum electrodynamics has proved elusive in experiments. Here we report neutron scattering measurements of the rare-earth pyrochlore magnet Pr$_2$Hf$_2$O$_7$ that provide evidence for a quantum spin ice ground state. We find a quasi-elastic structure factor with pinch points - a signature of a classical spin ice - that are partially suppressed, as expected in the quantum-coherent regime of the lattice field theory at finite temperature. Our result allows an estimate for the speed of light associated with magnetic photon excitations. We also reveal a continuum of inelastic spin excitations, which resemble predictions for the fractionalized, topological excitations of a quantum spin ice. Taken together, these two signatures suggest that the low-energy physics of Pr$_2$Hf$_2$O$_7$ can be described by emergent quantum electrodynamics. If confirmed, the observation of a quantum spin ice ground state would constitute a concrete example of a three-dimensional quantum spin liquid - a topical state of matter which has so far mostly been explored in lower dimensionalities.

cond-mat.str-el↗

arXiv2018

Exotic magnetic field-induced spin-superstructures in a mixed honeycomb triangular lattice system

The temperature-magnetic-field phase diagram of the mixed honeycomb triangular lattice system K$_{2}$Mn$_{3}$(VO$_{4}$)$_{2}$CO$_{3}$ is investigated by means of magnetization, heat capacity and neutron scattering measurements. The results indicate that triangular and honeycomb magnetic layers undergo sequential magnetic orderings and act as nearly independent magnetic sublattices. The honeycomb sublattice orders at about 85 K in a Neél-type antiferromagnetic structure, while the triangular sublattice displays two consecutive ordered states at much lower temperatures, 3 K and 2.2 K. The ground state of the triangular sublattice consists of a planar `Y' magnetic structure that emerges from an intermediate collinear `up-up-down' state. Applied magnetic fields parallel or perpendicular to the $c$-axis induce exotic ordered phases characterized by various spin-stacking sequences of triangular layers that yield bilayer, three-layer or four-layer magnetic superstructures. The observed superstructures cannot be explained in the framework of quasi-classical theory based only on nearest-neighbor interlayer coupling and point towards the presence of effective second-nearest-neighbor interactions mediated by fluctuations of the magnetic moments in the honeycomb sublattice.

cond-mat.str-el↗

arXiv2018

Neutron spin resonance as a probe of Fermi surface nesting and superconducting gap symmetry in Ba$_{0.67}$K$_{0.33}$(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$

We use inelastic neutron scattering to study energy and wave vector dependence of the superconductivity-induced resonance in hole-doped Ba$_{0.67}$K$_{0.33}$(Fe$_{1-x}$Co$_{x}$)$_{2}$As$_{2}$ ($x=0,0.08$ with $T_c\approx 37, 28$ K, respectively). In previous work on electron-doped Ba(Fe$_{0.963}$Ni$_{0.037}$)$_2$As$_2$ ($T_N=26$ K and $T_c=17$ K), the resonance is found to peak sharply at the antiferromagnetic (AF) ordering wave vector ${\bf Q}_{\rm AF}$ along the longitudinal direction, but disperses upwards away from ${\bf Q}_{\rm AF}$ along the transverse direction. For hole doped $x=0, 0.08$ without AF order, we find that the resonance displays ring-like upward dispersion away from ${\bf Q}_{\rm AF}$ along both the longitudinal and transverse directions. By comparing these results with calculations using the random phase approximation, we conclude that the dispersive resonance is a direct signature of isotropic superconducting gaps arising from nested hole-electron Fermi surfaces.

cond-mat.supr-con↗