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V. O. Garlea

Publications and source records attributed to V. O. Garlea.

At least 19 recordsLinked to original sources

Tunable inter-bilayer magnetic correlations and candidate multipolar physics in the van der Waals oxyhalides DyOCl, DyOBr, and DyOI

Rare-earth van der Waals magnets provide a route to combining strong spin-orbit coupling, large magnetic moments, and reduced dimensionality in bulk crystals. We report a comparative study of the dysprosium oxyhalides DyOX (X = Cl, Br, I), which realize square-bilayer networks of Dy3+ moments separated by a tunable van der Waals gap. Structural refinements show that increasing the halide ionic radius strongly expands the inter-bilayer spacing while leaving the local bilayer geometry nearly unchanged. Magnetization and heat-capacity measurements reveal two low-temperature anomalies in all three compounds: antiferromagnetic order at TN ~ 7-10 K and a broader anomaly near TQ ~ 27-30 K. Single-crystal magnetization on DyOCl and DyOBr establishes a strong hard-c-axis anisotropy, consistent with crystal-field analysis of DyOCl, which yields an XY-like ground-state g tensor. Neutron diffraction shows long-range antiferromagnetic order in DyOCl, whereas DyOBr and DyOI exhibit sharp magnetic scattering coexisting with Warren-like diffuse features, consistent with robust in-plane correlations and imperfect inter-bilayer registry. Inelastic neutron scattering on DyOCl identifies crystal-field excitations near 25-30 meV and an additional magnetic mode near 10 meV whose temperature dependence is tied to the high-temperature anomaly. Taken together, these results establish DyOX as a tunable family of quasi-two-dimensional rare-earth magnets and point to candidate multipolar physics associated with low-lying crystal-field states. Direct probes of quadrupolar order, such as resonant x-ray scattering or elastic-constant measurements, will be required to determine the order parameter at TQ.

cond-mat.str-el

Altermagnetic and dipolar splitting of magnons in FeF$_2$

FeF$_2$ is a prototypical rutile antiferromagnet recently proposed as an altermagnet, with a magnetic symmetry that permits spin-split electronic bands and chiral magnons. Using very-high-resolution inelastic neutron scattering on a single crystal of FeF$_2$, we show that the dominant source of magnon splitting is in fact the long-range dipolar interaction rather than altermagnetic exchange terms. At momenta where the dipolar splitting vanishes, we observe additional broadening due to altermagnetic chiral splitting and estimate this splitting to be $\sim$35 $μ$eV. Polarized measurements further reveal that, where dipolar splitting is present, the chiral magnon modes become mixed and the resulting modes are predominantly linearly polarized, with at most a small chiral component. These findings highlight the significant effect of dipolar interactions on magnon chirality, particularly when altermagnetic interactions are weak.

cond-mat.str-el

Magnetism of single crystalline breathing pyrochlore spinel AgInCr4S8

Single crystals of \ce{AgInCr4S8} were grown by chemical vapor transport and crystallographic ordering of Ag/In that results in a breathing pyrochlore motif of Cr$^{3+}$ was verified by x-ray and neutron diffraction. Long-range antiferromagnetic order is observed below a Néel temperature of $T_{\mathrm N}$ $\approx$ 9.6 K. The magnetic properties are characterized using ac and dc magnetization, specific heat capacity, and single crystal neutron diffraction measurements. The specific heat data are characterized by a small lambda anomaly near 9.5 K and the estimated magnetic entropy reaches $\approx$ $\frac{1}{3}$ of the expected value by 3$T_{\mathrm N}$, suggesting significant short-range order in the paramagnetic phase. Single crystal neutron diffraction evidences an incommensurate spin structure with propagation vector $\textbf{\textit{k}}$ = (0,0,$δ$) and $δ$ = 0.343 at 5 K. The minimal model that accounts for the data consists of ferromagnetic layers of Cr atoms, with magnetic moments lying in the plane of the layers and modulating in the perpendicular direction to form a helical structure propagating along $\textbf{\textit{k}}$. This study represents a rare investigation of single crystals within the family of breathing pyrochlore materials.

cond-mat.str-el

Localized Triplons and Site Stuffing in the Quantum Dimer Magnet BiYbGeO$_5$

Thermodynamic and muon spin-relaxation measurements have recently highlighted BiYbGeO$_5$ as a new example of a rare-earth-based quantum dimer magnet with isolated Yb$^{3+}$ spin-$\frac{1}{2}$ dimers. However, direct spectroscopic evidence of the triplet excitations and measurements of the structural disorder are lacking. In this work, polycrystalline BiYbGeO$_5$ was synthesized using conventional high-temperature solid-state methods and investigated via high-resolution neutron powder diffraction and inelastic neutron scattering. Diffraction measurements down to 58 mK reveal no signatures of magnetic order and indicate that nearly 20\% of Yb$^{3+}$ sites are replaced by non-magnetic Bi$^{3+}$, introducing significant structural disorder. Inelastic neutron scattering shows dispersionless triplon excitations, consistent with localized, non-interacting spin dimers. Fits to the triplet excitation spectrum identify an XXZ-type anisotropic exchange with $J_{XX}$ = 0.11(2) meV and $J_Z = 0.15(1)$ meV. These findings establish BiYbGeO$_5$ as a structurally disordered but magnetically well-isolated quantum dimer system, providing a model platform for studying the resilience of entangled spin states to site dilution.

cond-mat.str-el

Zig-Zag magnetic order and potential Kitaev interactions in the spin-1 honeycomb lattice KNiAsO$_4$

Despite the exciting implications of the Kitaev spin-Hamiltonian, finding and confirming the quantum spin liquid state has proven incredibly difficult. Recently the applicability of the model has been expanded through the development of a microscopic description of a spin-1 Kitaev interaction. Here we explore a candidate spin-1 honeycomb system, KNiAsO$_4$ , which meets many of the proposed criteria to generate such an interaction. Bulk measurements reveal an antiferromagnetic transition at $\sim$ 19 K which is generally robust to applied magnetic fields. Neutron diffraction measurements show magnetic order with a $\textbf{k}=(\frac{3}{2},0,0)$ ordering vector which results in the well-known ``zig-zag" magnetic structure thought to be adjacent to the spin-liquid ground state. Field dependent diffraction shows that while the structure is robust, the field can tune the direction of the ordered moment. Inelastic neutron scattering experiments show a well defined gapped spin-wave spectrum with no evidence of the continuum expected for fractionalized excitations. Modeling of the spin waves shows that the extended Kitaev spin-Hamiltonians is generally necessary to model the spectra and reproduce the observed magnetic order. First principles calculations suggest that the substitution of Pd on the Ni sublattice may strengthen the Kitaev interactions while simultaneously weakening the exchange interactions thus pushing KNiAsO$_4$ closer to the spin-liquid ground state.

cond-mat.str-el

Spin correlations in the frustrated ferro-antiferromagnet SrZnVO(PO4)2 near saturation

Single crystal elastic and inelastic neutron scattering experiments are performed on the frustrated ferro-antiferromagnet SrZnVO(PO4)2 in high magnetic fields. The fully polarized state, the presaturation phase and the columnar-antiferromagnetic phase just bellow the presaturation phase were investigated. The observed renormalization of spin wave bandwidths, re-distribution of intensities between different branches and non-linearities in the magnetization curve are all indicative of strong deviations from classical spin wave theory. The previously observed presaturation transition is attributed to a staggered pattern of Dzyaloshinskii-Moriya interactions.

cond-mat.str-el

Reinvestigation of crystal symmetry and fluctuations in La$_2$CuO$_4$

New surprises continue to be revealed about La$_2$CuO$_4$, the parent compound of the original cuprate superconductor. Here we present neutron scattering evidence that the structural symmetry is lower than commonly assumed. The static distortion results in anisotropic Cu-O bonds within the CuO$_2$ planes; such anisotropy is relevant to pinning charge stripes in hole-doped samples. Associated with the extra structural modulation is a soft phonon mode. If this phonon were to soften completely, the resulting change in CuO$_6$ octahedral tilts would lead to weak ferromagnetism. Hence, we suggest that this mode may be the "chiral" phonon inferred from recent studies of the thermal Hall effect. We also note the absence of interaction between the antiferromagnetic spin waves and low-energy optical phonons, in contrast to what is observed in hole-doped samples.

cond-mat.supr-con

Magnetic properties of the Shastry-Sutherland lattice material BaNd$_2$ZnO$_5$

We investigate the physical properties of the Shastry-Sutherland lattice material BaNd$_2$ZnO$_5$. Neutron diffraction, magnetic susceptibility, and specific heat measurements reveal antiferromagnetic order below 1.65 K. The magnetic order is found to be a 2-$\boldsymbol{Q}$ magnetic structure with the magnetic moments lying in the Shastry-Sutherland lattice planes comprising the tetragonal crystal structure of BaNd$_2$ZnO$_5$. The ordered moment for this structure is 1.9(1) $μ_B$ per Nd ion. Inelastic neutron scattering measurements reveal that the crystal field ground state doublet is well separated from the first excited state at 8 meV. The crystal field Hamiltonian is determined through simultaneous refinement of models with both the LS coupling and intermediate coupling approximations to the inelastic neutron scattering and magnetic susceptibility data. The ground state doublet indicates that the magnetic moments lie primarily in the basal plane with magnitude consistent with the size of the determined ordered moment.

cond-mat.str-el

Coexistence and interaction of spinons and magnons in an antiferromagnet with alternating antiferromagnetic and ferromagnetic quantum spin chains

In conventional quasi-one-dimensional antiferromagnets with quantum spins, magnetic excitations are carried by either magnons or spinons in different energy regimes: they do not coexist independently, nor could they interact with each other. In this Letter, by combining inelastic neutron scattering, quantum Monte Carlo simulations and Random Phase Approximation calculations, we report the discovery and discuss the physics of the coexistence of magnons and spinons and their interactions in Botallackite-Cu2(OH)3Br. This is a unique quantum antiferromagnet consisting of alternating ferromagnetic and antiferromagnetic Spin-1/2 chains with weak inter-chain couplings. Our study presents a new paradigm where one can study the interaction between two different types of magnetic quasiparticles, magnons and spinons.

cond-mat.str-el

Magnetic structure and exchange interactions in the layered semiconductor CrPS4

Compounds with two-dimensional (2D) layers of magnetic ions weakly connected by van der Waals bonding offer routes to enhance quantum behavior, stimulating both fundamental and applied interest. CrPS4 is one such magnetic van der Waals material, however, it has undergone only limited investigation. Here we present a comprehensive series of neutron scattering measurements to determine the magnetic structure and exchange interactions. The observed magnetic excitations allow a high degree of constraint on the model parameters not normally associated with measurements on a powder sample. The results demonstrate the 2D nature of the magnetic interactions, while also revealing the importance of interactions along 1D chains within the layers. The subtle role of competing interactions is observed, which manifest in a non-trivial magnetic transition and a tunable magnetic structure in a small applied magnetic field through a spin-flop transition. Our results on the bulk compound provide insights that can be applied to an understanding of the behavior of reduced layer CrPS4.

cond-mat.str-el

Crystal field Hamiltonian and anisotropy in KErSe2 and CsErSe2

We use neutron scattering and bulk property measurements to determine the single-ion crystal-field Hamiltonians of delafossites $\rm KErSe_2$ and $\rm CsErSe_2$. These two systems contains planar equilateral triangular Er lattices arranged in two stacking variants: rhombohedral (for K) or hexagonal (Cs). Our analysis shows that regardless the stacking order both compound exhibit an easy-plane ground state doublet with large $J_z=1/2$ terms and the potential for significant quantum effects, making them candidates for quantum spin liquid or other exotic ground states.

cond-mat.str-el

Van Hove singularity in the magnon spectrum of the antiferromagnetic quantum honeycomb lattice

The magnetic excitation spectrum of the quantum magnet YbCl$_3$ is studied with inelastic neutron scattering. The spectrum exhibits an unusually sharp feature within a broad continuum, as well as conventional spin waves. By including both transverse and longitudinal channels of the neutron response, linear spin wave theory with a single Heisenberg interaction on the honeycomb lattice reproduces all of the key features in the spectrum. In particular, the broad continuum corresponds to a two-magnon contribution from the longitudinal channel, while the sharp feature within this continuum is identified as a Van Hove singularity in the joint density of states, which indicates the two-dimensional nature of the two-magnon continuum. We term these singularities magneto-caustic features in analogy with caustic features in ray optics where focused envelopes of light are generated when light passes through or reflects from curved or distorted surfaces. The experimental demonstration of a sharp Van Hove singularity in a two-magnon continuum is important because analogous features in potential two-spinon continua could distinguish quantum spin liquids from merely disordered systems. These results establish YbCl$_3$ as a nearly ideal two-dimensional honeycomb lattice material hosting strong quantum effects in the unfrustrated limit.

cond-mat.str-el

Signatures of coupling between spin waves and Dirac fermions in YbMnBi$_2$

We present inelastic neutron scattering (INS) measurements of magnetic excitations in YbMnBi$_2$, which reveal features consistent with a direct coupling of magnetic excitations to Dirac fermions. In contrast with the large broadening of magnetic spectra observed in antiferromagnetic metals such as the iron pnictides, here the spin waves exhibit a small but resolvable intrinsic width, consistent with our theoretical analysis. The subtle manifestation of spin-fermion coupling is a consequence of the Dirac nature of the conduction electrons, including the vanishing density of states near the Dirac points. Accounting for the Dirac fermion dispersion specific to \ymb\ leads to particular signatures, such as the nearly wave-vector independent damping observed in the experiment.

cond-mat.str-el

Nature and impact of stripe freezing in La$_{1.67}$Sr$_{0.33}$NiO$_4$

La$_{1.67}$Sr$_{0.33}$NiO$_4$ develops charge and spin stripe orders at temperatures of roughly 200 K, with modulation wave vectors that are temperature independent. Various probes of spin and charge response have provided independent evidence for some sort of change below $\sim50$ K. In combination with a new set of neutron scattering measurements, we propose a unified interpretation of all of these observations in terms of a freezing of Ni-centered charges stripes, together with a glassy ordering of the spin stripes that shows up in neutron scattering as a slight rotation of the average spin direction.

cond-mat.str-el

Highly dispersive magnons with spin-gap like features in the frustrated ferromagnetic S=1/2 chain compound Ca2Y2Cu5O10 detected by inelastic neutron scattering

We report inelastic neutron scattering experiments in Ca2Y2Cu5O10 and map out the full one magnon dispersion which extends up to a record value of 53 meV for frustrated ferromagnetic (FM) edge-sharing CuO2 chain (FFESC) cuprates. A homogeneous spin-1/2 chain model with a FM nearest-neighbor (NN), an antiferromagnetic (AFM) next-nearest-neighbor (NNN) inchain, and two diagonal AFM interchain couplings (ICs) analyzed within linear spin-wave theory (LSWT) reproduces well the observed strong dispersion along the chains and a weak one perpendicularly. The ratio R=|J_{a2}/J_{a1}| of the FM NN and the AFM NNN couplings is found as ~0.23, close to the critical point Rc=1/4 which separates ferromagnetically and antiferromagnetically correlated spiral magnetic ground states in single chains, whereas Rc>0.25 for coupled chains is considerably upshifted even for relatively weak IC. Although the measured dispersion can be described by homogeneous LSWT, the scattering intensity appears to be considerably reduced at ~11.5 and ~28 meV. The gap-like feature at 11.5 meV is attributed to magnon-phonon coupling whereas based on DMRG simulations of the dynamical structure factor the gap at 28 meV is considered to stem partly from quantum effects due to the AFM IC. Another contribution is ascribed to the intrinsic superstructure from the distorting incommensurate pattern of CaY cationic chains adjacent to the CuO2 ones. It gives rise to non-equivalent CuO4 units and Cu-O-Cu bond angles Phi and a resulting distribution of all exchange integrals. The J's fitted by homogeneous LSWT are regarded as average values. The record value of the FM NN integral J1=24 meV among FFESC cuprates can be explained by a non-universal Phi (not 90 deg.) and Cu-O bond length dependent anisotropic mean direct FM Cu-O exchange K_{pd}~120 meV. Enhanced K_{pd} values are also needed to compensate a significant AFM J_{dd} > ~6 meV.

cond-mat.str-el

Crystal field splitting, local anisotropy, and low energy excitations in the quantum magnet YbCl$_3$

We study the correlated quantum magnet, YbCl$_3$, with neutron scattering, magnetic susceptibility, and heat capacity measurements. The crystal field Hamiltonian is determined through simultaneous refinements of the inelastic neutron scattering and magnetization data. The ground state doublet is well isolated from the other crystal field levels and results in an effective spin-1/2 system with local easy plane anisotropy at low temperature. Cold neutron spectroscopy shows low energy excitations that are consistent with nearest neighbor antiferromagnetic correlations of reduced dimensionality.

cond-mat.str-el

The magnetic order of a manganese vanadate system with two-dimensional striped triangular lattice

Results of magnetization and neutron diffraction measurements of the manganese vanadate system Mn$_5$(VO$_4$)$_2$(OH)$_4$ are reported. The crystal structure of this compound contains triangular [Mn$_3$O$_{13}$] building blocks that produce two-dimensional Mn$^{2+}$ magnetic networks with striped triangular topologies. The Mn sheets are connected through the nonmagnetic vanadate tetrahedra extending along the $a$-axis. Magnetization measurements performed on single crystals reveal the onset of a long-range antiferromagnetic order below approximately 45 K. The magnetic structure is Néel-type with nearest-neighbor Mn atoms coupled via three or four antiferromagnetic bonds. The magnetic moments are confined within the layers and are oriented parallel to the $b$ direction. The magnitudes of ordered moments are reduced, presumably by geometrical frustration and the low-dimensionality of the lattice structure.

cond-mat.str-el

Physical properties of the trigonal binary compound Nd$_2$O$_3$

We have studied the physical properties of Nd$_2$O$_3$ with neutron diffraction, inelastic neutron scattering, heat capacity, and magnetic susceptibility measurements. Nd$_2$O$_3$ crystallizes in a trigonal structure, with Nd$^{3+}$ ions surrounded by cages of 7 oxygen anions. The crystal field spectrum consists of four excitations spanning the energy range 3-60 meV. The refined eigenfunctions indicate XY-spins in the $ab$ plane. The Curie-Weiss temperature of $θ_{CW}=-23.7(1)$ K was determined from magnetic susceptibility measurements. Heat capacity measurements show a sharp peak at 550 mK and a broader feature centered near 1.5 K. Neutron diffraction measurements show that the 550 mK transition corresponds to long-range anti-ferromagnetic order implying a frustration index of $θ_{CW}/T_N\approx43$. These results indicate that Nd$_2$O$_3$ is a structurally and chemically simple model system for frustration caused by competing interactions with moments with predominate XY anisotropy.

cond-mat.str-el