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Douglas L. Abernathy

Publications and source records attributed to Douglas L. Abernathy.

At least 19 recordsLinked to original sources

Crystal electric field excitations and an effective-spin-$1/2$ ground doublet in the hyperkagome magnet Yb$_3$Sc$_2$Ga$_3$O$_{12}$

We use inelastic neutron scattering (INS) to determine the crystal electric field (CEF) excitations of Yb$^{3+}$ in the rare-earth hyperkagome magnet Yb$_3$Sc$_2$Ga$_3$O$_{12}$. Three nearly dispersionless magnetic excitations are observed near 58, 68, and 74~meV, corresponding to transitions from the ground-state Kramers doublet to the three excited doublets of the $J=7/2$ multiplet. A Stevens-operator analysis constrained by the local $222$ ($D_2$) symmetry reproduces the excitation energies and spectral weights and yields an Ising-type ground-state $g$ tensor. The first excited doublet lies approximately 58~meV above the ground state, establishing a well-isolated effective $J_{\mathrm{eff}}=1/2$ degree of freedom over the low-temperature regime relevant to collective magnetism. Notably, the directly measured CEF spectrum substantially revises the level scheme previously inferred from bulk measurements, while preserving the essential low-energy pseudospin description. Two independent fitting protocols give consistent excitation energies, ground-doublet wave functions, and $g$ tensors, despite the nonuniqueness of the individual CEF parameters. The resulting single-ion model also reproduces the characteristic susceptibility, magnetization, and field evolution of the Schottky anomaly in specific heat. These results establish the microscopic single-ion basis needed to construct an effective exchange Hamiltonian and to interpret future measurements of low-energy collective excitations in Yb$_3$Sc$_2$Ga$_3$O$_{12}$.

cond-mat.str-el↗

Emergent hidden order in ice: frustration and glassiness from slow hydrogen dynamics

Frustrated systems can host hidden order, in which weak interactions select correlated structure from a highly degenerate manifold. Water ice Ih is the canonical example of such a manifold, yet whether its hydrogen disorder conceals local structure beyond the Bernal-Fowler ice rules has remained controversial. Here, using high-resolution inelastic neutron scattering on single-crystal heavy ice, we identify strongly anisotropic librational phonons dispersing uniaxially along the crystallographic c axis - a spectroscopic signature inaccessible to bulk-averaging probes. A physics-guided analysis reveals that these excitations encode a hidden partial order: correlated polar armchair chains driven by a shallow stereochemical bias that creates an imperfectly flat energy landscape. This bias promotes nanoscale polar domains, yet frustrated topology prevents their straightforward coarsening into the ice XI ground state, trapping the system in a rugged configurational landscape that, within the experimentally constrained model, retains finite residual entropy even in the limit of infinitely slow cooling. These findings show that ice Ih is not a simple disordered solid, but a frustrated, partially ordered hydrogen network with glass-like arrest on a crystalline lattice, providing a microscopic framework that reconciles thermodynamic theory with spectroscopic observations.

cond-mat.mtrl-sci↗

Anisotropic magnons in a layered honeycomb ferromagnet

Recent experimental and theoretical studies have suggested a possible Dirac magnon gap in the two-dimensional ferromagnetic semiconductor CrSiTe$_3$. Detailed neutron scattering measurements were performed to shed light on the existence of the magnon gap, and suggest that the gap is very small or non-existent, with previous measurements being complicated by experimental factors. During these measurements, it was found that the out-of-plane couplings could explain the usual property of the increase in the magnetic transition temperature when CrSiTe$_3$ is exfoliated to monolayers. Furthermore, the material was shown to have anisotropic magnons along the out-of-plane direction, through the proposed Dirac point. We speculate that this is due to an exchange anisotropy, though Kitaev-like interactions alone cannot explain the spectra.

cond-mat.str-el↗

Nature of magnetism in bilayer nickelate La3Ni2O7 single crystals

The recent discovery of high-temperature superconductivity in pressurized and thin film nickelates has generated intense interest, yet the nature of magnetism in their ambient-pressure parent phases remains poorly understood, despite its potentially crucial role in pairing. Here we use neutron scattering to resolve the spin order and dynamics of single-crystalline La3Ni2O7, an ambient-pressure parent of this class. Well defined spin excitations are observed at Q = (0, 0.5, 2.5), featuring a~5 meV spin gap and anisotropic in-plane dispersions, with zone-boundary softening along the transverse direction indicative of competing exchange interactions. The excitations exhibit pronounced out-of-plane modulations with bilayer periodicity, providing direct evidence for antiferromagnetic interlayer coupling. Their dispersion is well described by a bilayer Heisenberg Hamiltonian with strong interlayer exchange and competing in-plane couplings within a stripe-type magnetic order. Normalization of the spectra to absolute units reveals that, although the spin-wave bandwidth is only about 25% of that in cuprates, the local dynamic susceptibility at comparable energies is significantly enhanced, yielding a total fluctuating moment of comparable magnitude. These results highlight intense mid-energy spin excitations rooted in substantial electronic correlations as a defining feature of this family, establishing a magnetic framework distinct from cuprates and directly relevant to understanding superconductivity in this system.

cond-mat.str-el↗

Uniaxial strain tuned magnetism of the altermagnet candidate h-FeS

Altermagnets are collinear magnetic materials with 'alter'nating local crystalline environments, characterized by joint spin and crystalline symmetries that enable ferromagnetic-like transport properties but with vanishing net magnetization. Hexagonal FeS (h-FeS) is a recently identified altermagnet candidate that shows a spontaneous anomalous Hall effect (AHE) accompanied by a tiny net magnetization. Here, we show that both the spontaneous AHE and magnetization can be effectively suppressed by an in-plane compressive strain. Since neutron diffraction measurements show that the applied uniaxial strain only modifies the in-plane domain population but does not affect the in-plane magnetic structure, the major effect of the applied strain is to tune the small $c$-axis ferromagnetic moment. Our results demonstrate a strong correlation between the tiny net magnetization and the spontaneous AHE in h-FeS, and show that uniaxial strain provides an effective knob to tune both properties in this altermagnet candidate for spintronic applications.

cond-mat.mtrl-sci↗

Complexity in the medium-range order of gallium as a polyvalent liquid metal

Simplicity in chemical composition does not always translate into simplicity in the structures and dynamics of liquids and solids. Some elementary liquid metals, such as gallium, show unusual behaviors in thermodynamic and transport properties as a result of their complex atomic structure and dynamics. In this work, we study the real-space atomic correlation function of liquid gallium by neutron scattering. In the pair-distribution function, there exist two kinds of medium-range order (MRO), characterized by oscillations beyond the first nearest neighbors. On the other hand, the first neighbor shell shows only one kind of bond. The two types of MRO are strongly overlapping in space and fluctuating in time. We propose that they are the basis for anomalous behavior of liquid gallium. This view challenges the current view that liquid gallium consists of fluctuating metallic and insulating domains. These findings shed new light on the interpretation of similar microscopic anomalies observed in other semi-metallic liquids.

cond-mat.soft↗

Real-space Atomic Dynamics in Liquid Gallium Studied by Inelastic Neutron Scattering

Gallium is a prototypical liquid metal and has gained renewed attention due to its unique properties. Characterizing and elucidating its atomic dynamics remains elusive despite numerous studies, primarily due to the challenges of quantifying atomic-scale dynamics in liquids. Recent developments in inelastic neutron scattering enable us to measure the Van Hove correlation function that describes the real-space motion of liquid atoms. In this work, we use this approach to reveal the dynamics in gallium liquids and find the co-existence of two dynamical medium-range orders (MROs), which have a dynamical behavior distinct from that of the short-range order (SRO). We propose that these MROs are driven by global forces in the form of two density waves, as a direct consequence of the underlying competition between ionic core repulsion and valence electron cohesion. We suggest that the density wave approach is not only applicable to other metallic liquids exhibiting similar structural anomalies, but also offers a promising direction for elucidating the dynamics of complex liquids and glasses by linking electronic-state fluctuations to atomic dynamics.

cond-mat.soft↗

Spin dynamics in itinerant antiferromagnet SrCr$_2$As$_2$

SrCr$_2$As$_2$ is an itinerant antiferromagnet in the same structural family as the SrFe$_2$As$_2$ high-temperature superconductors. We report our calculations of exchange-coupling parameters $J_{ij}$ for SrCr$_2$As$_2$ using a static linear-response method based on first-principles electronic-structure calculations. We find that the dominant nearest-neighbor exchange coupling $J_{\rm{1}} > 0$ is antiferromagnetic whereas the next-nearest-neighbor interaction $J_{\rm{2}} < 0$ is ferromagnetic with $J_{\rm{2}}$/$J_{\rm{1}}$~=~$-0.68$, reinforcing the checkerboard in-plane magnetic structure. Thus, unlike other transition-metal arsenides based on Mn, Fe, or Co, we find no competing magnetic interactions in SrCr$_2$As$_2$, which aligns with experimental findings. Moreover, the orbital resolution of exchange interactions shows that $J_1$ and $J_2$ are dominated by direct exchange mediated by the Cr $d$ orbitals. To validate the calculations we conduct inelastic neutron-scattering measurements on powder samples that show steeply dispersive magnetic excitations arising from the magnetic $Γ$ points and persisting up to energies of at least 175 meV. The spin-wave spectra are then modeled using the Heisenberg Hamiltonian with the theoretically-calculated exchange couplings. The calculated neutron-scattering spectra are in good agreement with the experimental data.

cond-mat.supr-con↗

Anomalous Electrical Transport in the Kagome Magnet YbFe$_6$Ge$_6$

Two-dimensional (2D) kagome metals offer a unique platform for exploring electron correlation phenomena derived from quantum many-body effects. Here, we report a combined study of electrical magnetotransport and neutron scattering on YbFe$_6$Ge$_6$, where the Fe moments in the 2D kagome layers exhibit an $A$-type collinear antiferromagnetic order below $T_{\rm{N}} \approx 500$ K. Interactions between the Fe ions in the layers and the localized Yb magnetic ions in between reorient the $c$-axis aligned Fe moments to the kagome plane below $T_{\rm{SR}} \approx 63$ K. Our magnetotransport measurements show an intriguing anomalous Hall effect (AHE) that emerges in the spin-reorientated collinear state, accompanied by the closing of the spin anisotropy gap as revealed from inelastic neutron scattering. The gapless spin excitations and the Yb-Fe interaction are able to support a dynamic scalar spin chirality, which explains the observed AHE. Therefore, our study demonstrates spin fluctuations may provide an additional scattering channel for the conduction electrons and give rise to AHE even in a collinear antiferromagnet.

cond-mat.str-el↗

Crystal field splittings and magnetic ground state of the square-lattice antiferromagnets YbBi2ClO4 and YbBi2IO4 with Jeff = 1/2

We report on the crystal field level splitting and magnetic ground state of the Jeff = 1/2 square lattice antiferromagnets YbBi2ClO4 and YbBi2IO4 using powder inelastic neutron scattering (INS) and neutron diffraction measurements. Both compounds exhibit a well-isolated $Γ_{7}$ doublet ground state under a tetragonal crystal field environment, confirming a robust Jeff = 1/2 picture with slight XY-type anisotropic character in the g-tensor. Notably, the ground state wave functions closely resemble the $Γ_{7}$ doublet expected in the perfect cubic limit, consistent with the nearly cubic ligand configuration of eight O2- ions surrounding Yb3+. Below TN =0.21 K, YbBi2IO4 exhibits a stripe long-range magnetic order characterized by an ordering wave vector qm = (1/2, 0, 0) or its symmetry-equivalent (0, 1/2, 0), with magnetic moments aligned along qm. The ordered moment is approximately 79 % of the classical prediction, significantly larger than expected from the isotropic J1-J2 model, suggesting the possible involvement of exchange anisotropy in explaining this observation. We show that symmetry-allowed XXZ and bond-dependent anisotropic exchange terms in a square lattice can play a critical role in stabilizing the stripe order and suppressing the moment reduction as observed. These findings establish YbBi2ClO4 and YbBi2IO4 as unique platforms for exploring rich Jeff = 1/2 magnetism from two less investigated perspectives: (i) on a square lattice and (ii) within a (nearly) cubic ligand environment.

cond-mat.str-el↗

Gapped commensurate antiferromagnetic response in a strongly underdoped model cuprate superconductor

It is a distinct possibility that spin fluctuations are the pairing interactions in a wide range of unconventional superconductors. In the case of the high-transition-temperature (high-$T_c$) cuprates, in which superconductivity emerges upon doping an antiferromagnetic Mott-insulating state, spin correlations might furthermore drive unusual pseudogap phenomena. Here we use polarized and unpolarized magnetic neutron scattering to study the simple tetragonal cuprate $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$ at very low doping ($T_c \approx 55$ K, hole concentration $p \approx 0.064$). In stark contrast to prior results for other underdoped cuprates, we find no evidence of incommensurate spin-density-wave, charge-spin stripe, or $q = 0$ magnetic order. Instead, the antiferromagnetic response in both the superconducting and pseudogap states is gapped below $Δ_\mathrm{AF} \approx 6$ meV, commensurate over a wide energy range, and disperses above about 55 meV. Given the documented model nature of $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$, which exhibits high structural symmetry and minimal point disorder effects, we conclude that the observed behavior signifies the unmasked response of the quintessential $\mathrm{CuO}_{2}$ planes near the Mott-insulating state. These results for $\mathrm{HgBa}_{2}\mathrm{CuO}_{4+δ}$ can therefore be expected to serve as a benchmark for a refined theoretical understanding of the cuprates.

cond-mat.supr-con↗

Dynamic crystallography reveals spontaneous anisotropy in cubic GeTe

Cubic energy materials such as thermoelectrics or hybrid perovskite materials are often understood to be highly disordered. In GeTe and related IV-VI compounds, this is thought to provide the low thermal conductivities needed for thermoelectric applications. Since conventional crystallography cannot distinguish between static disorder and atomic motions, we develop the energy-resolved variable-shutter pair distribution function technique. This collects structural snapshots with varying exposure times, on timescales relevant for atomic motions. In disagreement with previous interpretations, we find the time-averaged structure of GeTe to be crystalline at all temperatures, but with anisotropic anharmonic dynamics at higher temperatures that resemble static disorder at fast shutter speeds, with correlated ferroelectric fluctuations along the $<$100$>$c direction. We show that this anisotropy naturally emerges from a Ginzburg-Landau model that couples polarization fluctuations through long-range elastic interactions. By accessing time-dependent atomic correlations in energy materials, we resolve the long-standing disagreement between local and average structure probes, and show that spontaneous anisotropy is ubiquitous in cubic IV-VI materials.

cond-mat.mtrl-sci↗

Diffusive Excitonic Bands from Frustrated Triangular Sublattice in a Singlet-Ground-State System

Magnetic order in most materials occurs when magnetic ions with finite moments in a crystalline lattice arrange in a particular pattern below the ordering temperature determined by exchange interactions between the ions. However, when the crystal electric field (CEF) effect results in a spin-singlet ground state on individual magnetic sites, the collective ground state of the system can either remain non-magnetic, or more intriguingly, the exchange interactions between neighboring ions, provided they are sufficiently strong, can admix the excited CEF levels, resulting in a magnetically ordered ground state. The collective magnetic excitations in such a state are so-called spin excitons that describe the CEF transitions propagating through the lattice. In most cases, spin excitons originating from CEF levels of a localized single ion are dispersion-less in momentum (reciprocal) space and well-defined in both the magnetically ordered and paramagnetic states. Here we use thermodynamic and neutron scattering experiments to study stoichiometric Ni2Mo3O8 without site disorder, where Ni2+ ions form a bipartite honeycomb lattice comprised of two triangular lattices, with ions subject to the tetrahedral and octahedral crystalline environment, respectively. We find that in both types of ions, the CEF excitations have nonmagnetic singlet ground states, yet the material has long-range magnetic order. Furthermore, CEF spin excitons from the triangular-lattice arrangement of tetrahedral sites form, in both the antiferromagnetic and paramagnetic states, a dispersive diffusive pattern around the Brillouin zone boundary in reciprocal space. The present work thus demonstrates that spin excitons in an ideal triangular lattice magnet can have dispersive excitations, irrespective of the existence of static magnetic order, and this phenomenon is most likely due to spin entanglement and geometric frustrations.

cond-mat.str-el↗

Frustration-induced diffusive scattering anomaly and dimension change in $\rm FeGe_2$

Magnetic frustration, arising from the competition of exchange interactions, has received great attention because of its relevance to exotic quantum phenomena in materials. In the current work, we report an unusual checkerboard-shaped scattering anomaly in $\rm FeGe_2$, far from the known incommensurate magnetic satellite peaks, for the first time by inelastic neutron scattering. More surprisingly, such phenomenon appears as spin dynamics at low temperature, but it becomes prominent above Néel transition as elastic scattering. A new model Hamiltonian that includes an intraplane next-nearest neighbor was proposed and attributes such anomaly to the near-perfect magnetic frustration and the emergence of unexpected two-dimensional magnetic order in the quasi-one-dimensional $\rm FeGe_2$.

cond-mat.mtrl-sci↗

Electronic and structural properties of RbCeX$_2$ (X$_2$: O$_2$, S$_2$, SeS, Se$_2$, TeSe, Te$_2$)

Triangular lattice delafossite compounds built from magnetic lanthanide ions are a topic of recent interest due to their frustrated magnetism and realization of quantum disordered magnetic ground states. Here we report the evolution of the structure and electronic ground states of RbCe$X_2$ compounds, built from a triangular lattice of Ce$^{3+}$ ions, upon varying their anion character ($X_2$= O$_2$, S$_2$, SeS, Se$_2$, TeSe, Te$_2$). This includes the discovery of a new member of this series, RbCeO$_2$, that potentially realizes a quantum disordered ground state analogous to NaYbO$_2$. Magnetization and susceptibility measurements reveal that all compounds manifest mean-field antiferromagnetic interactions and, with the exception of the oxide, possess signatures of magnetic correlations onset below 1 K. The crystalline electric field level scheme is explored via neutron scattering and \textit{ab initio} calculations in order to model the intramultiplet splitting of the $J=5/2$ multiplet. In addition to the two excited doublets expected within the $J=5/2$ manifold, we observe one extra, local mode present across the sample series. This added mode shifts downward in energy with increasing anion mass and decreasing crystal field strength, suggesting a long-lived anomalous mode endemic to anion motion about the Ce$^{3+}$ sites.

cond-mat.str-el↗

Neutron Scattering Signature of Phonon Renormalization in Nickel (II) Oxide

The physics of mutual interaction of phonon quasiparticles with electronic spin degrees of freedom, leading to unusual transport phenomena of spin and heat, has been a subject of continuing interests for decades. Despite its pivotal role in transport processes, the effect of spin-phonon coupling on the phonon system, especially acoustic phonon properties, has so far been elusive. By means of inelastic neutron scattering and first-principles calculations, anomalous scattering spectral intensity from acoustic phonons was identified in the exemplary collinear antiferromagnetic nickel (II) oxide, unveiling strong spin-lattice correlations that renormalize the polarization of acoustic phonon. In particular, a clear magnetic scattering signature of the measured neutron scattering intensity from acoustic phonons is demonstrated by its momentum transfer and temperature dependences. The anomalous scattering intensity is successfully modeled with a modified magneto-vibrational scattering cross section, suggesting the presence of spin precession driven by phonon. The renormalization of phonon eigenvector is indicated by the observed "geometry-forbidden" neutron scattering intensity from transverse acoustic phonon. Importantly, the eigenvector renormalization cannot be explained by magnetostriction but instead, it could result from the coupling between phonon and local magnetization of ions.

cond-mat.mtrl-sci↗

High Phonon Scattering Rates Suppress Thermal Conductivity in Hyperstoichiometric Uranium Dioxide

Uranium dioxide (UO$_2$), one of the most important nuclear fuels, can accumulate excess oxygen atoms as interstitial defects, which significantly impacts thermal properties. In this study, thermal conductivities and inelastic neutron scattering measurements on UO$_2$ and UO$_{2+x}$ (x=0.3, 0.4, 0.8, 0.11) were performed at low temperatures (2-300 K). The thermal conductivity of UO$_{2+x}$ is significantly suppressed compared to UO$_2$ except near the Néel temperature TN= 30.8 K, where it is independent of x. Phonon measurements demonstrate that the heat capacities and phonon group velocities of UO$_2$ and UO$_{2+x}$ are similar and that the suppressed thermal conductivity in UO$_{2+x}$ results from high phonon scattering rates. These new insights advance our fundamental understanding of thermal transport properties in advanced nuclear fuels.

cond-mat.mtrl-sci↗

Spiral spin-liquid on a honeycomb lattice

Spiral spin-liquids are correlated paramagnetic states with degenerate propagation vectors forming a continuous ring or surface in reciprocal space. On the honeycomb lattice, spiral spin-liquids present a novel route to realize emergent fracton excitations, quantum spin liquids, and topological spin textures, yet experimental realizations remain elusive. Here, using neutron scattering, we show that a spiral spin-liquid is realized in the van der Waals honeycomb magnet FeCl$_3$. A continuous ring of scattering is directly observed, which indicates the emergence of an approximate U(1) symmetry in momentum space. Our work demonstrates that spiral spin-liquids can be achieved in two-dimensional systems and provides a promising platform to study the fracton physics in spiral spin-liquids.

cond-mat.str-el↗