The Kitaev quantum spin liquid epitomizes an entangled topological state, for which two flavors of fractionalized low-energy excitations are predicted: the itinerant Majorana fermion and the Z 2 gauge flux. Here, it was proposed recently that fingerprints of fractional excitations are encoded in the phonon spectra of Kitaev quantum spin liquids through a novel fractional-excitation-phonon coupling. Here, we detect anomalous phonon effects in α-RuCl 3 using inelastic X-ray scattering with meV resolution. At high temperature, we discover interlaced optical phonons intercepting a transverse acoustic phonon between 3 and 7 meV. Upon decreasing temperature, the optical phonons display a large intensity enhancement near the Kitaev energy, J K ~8 meV, that coincides with a giant acoustic phonon softening near the Z 2 gauge flux energy scale. These phonon anomalies signify the coupling of phonon and Kitaev magnetic excitations in α-RuCl 3 and demonstrates a proof-of-principle method to detect anomalous excitations in topological quantum materials.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Magnetic exchange interactions in the van der Waals layered antiferromagnet MnPSe 3

Two-dimensional van der Waals compounds with magnetic ions on a honeycomb lattice are hosts to a variety of exotic behavior. The magnetic interactions in one such compound, MnPSe 3 , are investigated with elastic and inelastic neutron scattering. Magnetic excitations are observed in the magnetically ordered regime and persist to temperatures well above the ordering temperature, T N =74K, consistent with low dimensional magnetic interactions. The inelastic neutron scattering results allow a model spin Hamiltonian to be presented that includes dominant intralayer interactions of J 1ab =0.45 meV, J 2ab =0.03 meV, J 3ab =0.19 meV, consistent with theoretical predictions. Furthermore, despite the quasi-2D behavior, appreciable interlayer interactions of J c =0.031(5) meV are required to model the data. No evidence for anisotropy in the form of a spin gap is observed in the data collected. The measurements on MnPSe 3 are contrasted with those on MnPS 3 and reveal a large increase in the interlayer exchange interaction in MnPSe 3 that may stabilize the similar ordering temperatures in the bulk compounds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Canted antiferromagnetic order in the monoaxial chiral magnets V 1/3 TaS 2 and V 1/3 NbS 2

The Dzyaloshinskii-Moriya (DM) interaction is present in the transition metal dichalcogenides (TMDC) magnets of form M 1 / 3 T S 2 ( M = 3 d transition metal, T ϵ { Nb , Ta } ), given that the intercalants M form 3 × 3 superlattices within the structure of the parent materials T S 2 and break the centrosymmetry. Competition between DM and ferromagnetic exchange interactions has been shown to stabilize a topological defect known as a chiral soliton in select intercalated TMDCs, initiating interest both in terms of fundamental physics and the potential for technological applications. In the current article we report on our study of the materials V 1 / 3 TaS 2 and V 1 / 3 NbS 2 , using a combination of x-ray powder diffraction, magnetization, and single crystal neutron diffraction. Historically identified as ferromagnets, our diffraction results instead reveal that vanadium spins in these compounds are arranged into an A-type antiferromagnetic configuration at low temperatures. Refined moments are 1.37(6) and 1.50(9) μ B for V 1 / 3 TaS 2 and V 1 / 3 NbS 2 , respectively. Transition temperatures T c = 32 K for V 1 / 3 TaS 2 and 50 K for V 1 / 3 NbS 2 are obtained from the magnetization and neutron diffraction results. We attribute the small net magnetization observed in the low-temperature phases to a subtle ( ~ 2 ° ) canting of XY spins in the out-of-plane direction. These new results are indicative of dominant antiferromagnetic exchange interactions between the vanadium moments in adjacent a b planes, likely eliminating the possibility of identifying stable chiral solitons in the current materials.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Robust cycloid crossover driven by anisotropy in the skyrmion host GaV 4 S 8

We report on the anomalous magnetization dynamics of the cycloidally modulated spin textures under the influence of uniaxial anisotropy in multiferroic GaV 4 S 8 . The temperature and field dependence of the linear ac susceptibility [$χ'_{1ω}$ (T, H)], AC magnetic loss [$χ''_{1ω}$ (T, H)], and nonlinear AC magnetic response [$M_{3ω}$ (T, H)] are examined across the magnetic phase diagram in the frequency range f = 10 - 10 000 Hz. According to recent theory, skyrmion vortices under axial crystal symmetry are confined along specific orientations, resulting in enhanced robustness against oblique magnetic fields and altered spin dynamics. We characterize the magnetic response of each spin texture and find that the dynamic rigidity of the Néel skyrmion lattice appears enhanced compared to Bloch-type skyrmions in cubic systems, even in the multidomain state. Anomalous M 3 ω and strong dissipation emerge over the same phase regime where strong variations in the cycloid pitch were observed on lowering temperature in recent small-angle neutron-scattering experiments [White et al., Phys. Rev. B 97, 020401(R) (2018)]. Here, we show that strong anisotropy also drives an extended crossover of the zero-field cycloid texture in GaV 4 S 8 . The frequency dependence of these dynamic signatures is consistent with that of a robust anharmonic spin texture exhibiting a correlated domain arrangement. The results underpin the essential role of magnetic anisotropy in enhancing the rigidity of topological spin textures for diverse applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Spin and orbital excitations through the metal-to-insulator transition in Cd 2 Os 2 O 7 probed with high-resolution resonant inelastic x-ray scattering

Here, high-resolution resonant inelastic x-ray scattering measurements (ΔE=46meV) have been performed on Cd 2 Os 2 O 7 through the metal-to-insulator transition (MIT). A magnetic excitation at 125 meV evolves continuously through the MIT, in agreement with recent Raman-scattering results, and provides further confirmation for an all-in all-out magnetic ground state. Asymmetry of this feature is likely a result of coupling between the electronic and the magnetic degrees of freedom. We also observe a broad continuum of interband excitations centered at 0.3 eV energy loss. This is indicative of significant hybridization between Os 5d and O 2p states and the concurrent itinerant nature of the system. In turn, this suggests a possible breakdown of the free-ion model for Cd 2 Os 2 O 7 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2019

V 51 -NMR study on the S = 1 2 square lattice antiferromagnet K 2 V 3 O 8

Not Available

Takeda, H. (ORCID:0000000207260601)↗

DOE OSTI2018

Field evolution of magnons in α - RuCl 3 by high-resolution polarized terahertz spectroscopy

Here, the Kitaev quantum spin liquid (KSL) is a theoretically predicted state of matter whose fractionalized quasiparticles are distinct from bosonic magnons, the fundamental excitation in ordered magnets. The layered honeycomb antiferromagnet α–RuCl 3 is a KSL candidate material, as it can be driven to a magnetically disordered phase by application of an in-plane magnetic field, with H c ~ 7 T. Here, we report a detailed characterization of the magnetic excitation spectrum of this material by high-resolution time-domain terahertz spectroscopy. We observe two sharp magnon resonances whose frequencies and amplitudes exhibit a discontinuity as a function of applied magnetic field, as well as two broader peaks at higher energy. Below the Néel temperature, we find that linear spin wave theory can account for all of these essential features of the spectra when a C 3 -breaking distortion of the honeycomb lattice and the presence of structural domains are taken into account.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Anisotropic susceptibilities in the honeycomb Kitaev system α - RuCl 3

The magnetic insulator α - RuCl 3 is a promising candidate to realize Kitaev interactions on a quasi-two-dimensional honeycomb lattice. We perform extensive susceptibility measurements on single crystals of α - RuCl 3 , including angle dependence of the in-plane longitudinal and transverse susceptibilities, which reveal a unidirectional anisotropy within the honeycomb plane. By comparing the experimental results to a high-temperature expansion of a Kitaev-Heisenberg-$\textbf{Γ}$ spin Hamiltonian with bond anisotropy, we find excellent agreement with the observed phase shift and periodicity of the angle-resolved susceptibilities. Within this model, we show that the pronounced difference between in-plane and out-of-plane susceptibilities as well as the finite transverse susceptibility are rooted in strong symmetric off-diagonal $\textbf{Γ}$ spin exchange. The $\textbf{Γ}$ couplings and relationships between other terms in the model Hamiltonian are quantified by extracting relevant Curie-Weiss intercepts from the experimental data.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Publisher Correction: Strongly-coupled quantum critical point in an all-in-all-out antiferromagnet

The original PDF version of the Article contained an error in the last sentence of the author affiliation information, which incorrectly read ‘Correspondence and requests for materials should be addressed to T.$.R. (e-mail: tfr@caltech.edu) or to Y.F. (e-mail: yejun@oist.jp)’. The correct version states ‘T.F.R.’ in place of “T.$.R.’. This has been corrected in the PDF version of the Article. The HTML version was correct from the time of publication.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Strongly-coupled quantum critical point in an all-in-all-out antiferromagnet

Dimensionality and symmetry play deterministic roles in the laws of Nature. They are important tools to characterize and understand quantum phase transitions, especially in the limit of strong correlations between spin, orbit, charge, and structural degrees of freedom. Using newly-developed, high-pressure resonant x-ray magnetic and charge diffraction techniques, we have discovered a quantum critical point in Cd 2 Os 2 O 7 as the all-in-all-out antiferromagnetic order is continuously suppressed to zero temperature and, concomitantly, the cubic lattice structure continuously changes from space group Fd-3m to F-43m. Surrounded by three phases of different time reversal and spatial inversion symmetries, the quantum critical region anchors two phase lines of opposite curvature, with striking departures from a mean-field form at high pressure. As spin fluctuations, lattice breathing modes, and quasiparticle excitations interact in the quantum critical region, we argue that they present the necessary components for strongly-coupled quantum criticality in this three-dimensional compound.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Extended exchange interactions stabilize long-period magnetic structures in Cr 1/3 NbS 2

The topologically protected, chiral soliton lattice is a unique state of matter offering intriguing functionality, and it may serve as a robust platform for storing and transporting information in future spintronic devices. While the monoaxial chiral magnet Cr 1/3 NbS 2 is known to host this exotic state in an applied magnetic field, its detailed microscopic origin has remained a matter of debate. In this paper, we work towards addressing this open question by measuring the spin wave spectrum of Cr 1/3 NbS 2 over the entire Brillouin zone with inelastic neutron scattering. The well-defined spin wave modes allow us to determine the values of several microscopic interactions for this system. The experimental data are well-explained by a Heisenberg Hamiltonian with exchange constants up to the third nearest neighbor and an easy plane magnetocrystalline anisotropy term. Finally, our work shows that both the second and third nearest neighbor exchange interactions contribute to the formation of the helimagnetic and chiral soliton lattice states in this robust three-dimensional magnet.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2018

LaCu 6 − x Ag x : A promising host of an elastic quantum critical point

Not Available

Poudel, L.↗

DOE OSTI2018

Negative thermal expansion and magnetoelastic coupling in the breathing pyrochlore lattice material LiGaCr 4 S 8

In this paper, the physical properties of the spinel LiGaCr 4 S 8 have been studied with neutron diffraction, x-ray diffraction, magnetic susceptibility, and heat capacity measurements. The neutron diffraction and synchrotron x-ray diffraction data reveal negative thermal expansion (NTE) below 111(4) K. The magnetic susceptibility deviates from Curie-Weiss behavior with the onset of NTE. At low temperature a broad peak in the magnetic susceptibility at 10.3(3) K is accompanied by the return of normal thermal expansion. First-principles calculations find a strong coupling between the lattice and the simulated magnetic ground state. Finally, these results indicate strong magnetoelastic coupling in LiGaCr 4 S 8 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗