arXiv subjects

Robert J. McQueeney

Publications and source records attributed to Robert J. McQueeney.

At least 19 recordsLinked to original sources

arXiv2025

Hidden symmetry-breaking in a kagome Ising ferromagnet

Kagome metals can host unconventional electronic phenomena that emerge from their frustrated lattice geometry and associated band topology. Correlated electronic orders, such as charge-density waves and superconductivity, are observed to intertwine with subtle time-reversal symmetry breaking whose microscopic origin is not currently understood. Here, we provide evidence for such time-reversal symmetry breaking in the kagome metal TbV$_6$Sn$_6$ arising from staggered magnetic moments within the kagome layers. TbV$_6$Sn$_6$ consists of metallic V kagome layers separated by Tb triangular layers that host Ising ferromagnetic order. Deep in the ferromagnetic state, the Tb Ising doublet ground state should display a single, dispersionless spin-flip excitation. Instead, inelastic neutron scattering reveals two sharp excitations associated with inequivalent Tb sites, demonstrating that a symmetry-broken phase coexists with Ising ferromagnetism. No additional structural or magnetic phase transitions are detected, and first-principles calculations rule out lattice distortions as the origin of the splitting. We attribute this effect to time-reversal symmetry breaking encoded by small V moments that couple to the Tb sublattice and leave a measurable spectral fingerprint. Our results establish rare-earth local moment spectroscopy as a sensitive probe of subtle broken symmetries and highlight an unexpected interplay between kagome magnetism and rare-earth local moment magnetism.

cond-mat.str-el↗

arXiv2025

Observation of the Axion quasiparticle in 2D MnBi$_2$Te$_4$

In 1978, Wilczek and Weinberg theoretically discovered a new boson-the Axion-which is the coherent oscillation of the $θ$ field in QCD. Its existence can solve multiple fundamental questions including the strong CP problem of QCD and the dark matter. However, its detection is challenging because it has almost no interaction with existing particles. Similar $θ$ has been introduced to condensed matter and so far studied as a static, quantized value to characterize topology of materials. But the coherent oscillation of $θ$ in condensed matter is proposed to lead to new physics directly analogous to the high-energy Axion particle, the dynamical Axion quasiparticle (DAQ). In this paper, we present the direct observation of the DAQ. By combining 2D electronic device with ultrafast pump-probe optics, we manage to measure the magnetoelectric coupling $θ$ ($θ\proptoα$) of 2D MnBi$_2$Te$_4$ with sub-picosecond time-resolution. This allows us to directly observe the DAQ by seeing a coherent oscillation of $θ$ at ~44 GHz in real time, which is uniquely induced by the out-of-phase antiferromagnetic magnon. Interestingly, in 2D MnBi$_2$Te$_4$, the DAQ arises from the magnon-induced coherent modulation of Berry curvature. Such ultrafast control of quantum wavefunction can be generalized to manipulate Berry curvature and quantum metric of other materials in ultrafast time-scale. Moreover, the DAQ enables novel quantum physics such as Axion polariton and electric control of ultrafast spin polarization, implying applications in unconventional light-matter interaction and coherent antiferromagnetic spintronics. Beyond condensed matter, the DAQ can serve as a detector of the dark matter Axion particle. We estimate the detection frequency range and sensitivity in the critically-lacking meV regime, contributing to one of the most challenging questions in fundamental physics.

cond-mat.mes-hall↗

arXiv2025

Design and Predict Tetragonal van der Waals Layered Quantum Materials of MPd$_5$I$_2$ (M=Ga, In and 3$d$ Transition Metals)

Quantum materials with stacked van der Waals (vdW) layers hosting non-trivial band structure topology and magnetism have shown many interesting properties. Using high throughput density functional theory calculations, we design and predict tetragonal vdW-layered quantum materials in the MPd$_5$I$_2$ structure (M=Ga, In and 3d transition metals). We show that besides the known AlPd$_5$I$_2$, the -MPd$_5$- structural motif of three-atomic-layer slabs separated by two I layers can accommodate a variety of metal atoms giving arise to topologically non-trivial features and highly tunable magnetic properties in both bulk and single layer 2D structures. Among them, TiPd$_5$I$_2$ and InPd$_5$I$_2$ host a pair of Dirac points and likely an additional strong topological insulator state for the band manifolds just above and below the top valence band, respectively, with their single layers hosting or near quantum spin Hall states. CrPd$_5$I$_2$ is a ferromagnet with a large out-of-plane magneto-anisotropy energy, desirable for rare-earth-free permanent magnets.

cond-mat.mtrl-sci↗

arXiv2025

Spiral Spin Liquid State in the Corrugated Honeycomb Lattice of CaMn$_2$P$_2$

CaMn$_2$P$_2$ exemplifies the realization of a frustrated $J_1$-$J_2$-$J_3$ Heisenberg model of a corrugated honeycomb magnetic lattice. Previous studies show that below the Néel temperature ($T_{\rm N}$), the system forms a cycloidal $6\times 6$ $ab$-plane magnetic unit cell that conforms with various magnetic space groups. Here, we present single-crystal neutron-diffraction studies across expansive reciprocal-space volumes, confirming the cycloidal magnetic structure while uncovering further distinctive features. We find evidence for three magnetic domains, the analysis of which narrows the possible magnetic model structures. At $T_{\rm N}$, the insulator exhibits a sharp phase transition, above which the spin structure transforms into a spiral spin liquid state, evident via a continuous ring of scattering with degenerate wavevectors corresponding to a collection of short-range spiral spin configurations. These degenerate states emerge as thermal fluctuations effectively reduce the $J_3$ interaction. The integration of experimental, theoretical, and real-space simulation results reveals the intricate balance of exchange interactions ($J_1$-$J_2$-$J_3$) that stabilizes the ground-state magnetic structure and drives the emergence of a sought-after $U$(1)-symmetric spiral spin-liquid state with easy-plane anisotropy above the transition temperature.

cond-mat.str-el↗

arXiv2024

Magnetic interactions and excitations in SrMnSb$_2$

The magnetic interactions in the antiferromagnetic (AFM) Dirac semimetal candidate SrMnSb$_2$ are investigated using \textit{ab initio} linear response theory and inelastic neutron scattering (INS). Our calculations reveal that the first two nearest in-plane couplings ($J_1$ and $J_2$) are both AFM in nature, indicating a significant degree of spin frustration, which aligns with experimental observations. The orbital resolution of exchange interactions shows that $J_1$ and $J_2$ are dominated by direct and superexchange, respectively. In a broader context, a rigid-band model suggests that electron doping fills the minority spin channel and results in a decrease in the AFM coupling strength for both $J_1$ and $J_2$. To better compare with INS measurements, we calculate the spin wave spectra within a linear spin wave theory, utilizing the computed exchange parameters. Although the calculated spin wave spectra somewhat overestimate the magnon bandwidth, they exhibit overall good agreement with measurements from INS experiments.

cond-mat.mtrl-sci↗

arXiv2024

Coexistence of Ferromagnetism and Antiferromagnetic Dimers in Topological Insulators

The addition of magnetic impurities in topological insulators can drive ferromagnetic order that leads to novel quantum anomalous Hall transport well below the Curie temperature. The fragility of the quantized regime has been ascribed to the random nature of the magnetic moment distribution. Here, we refine this hypothesis by using inelastic neutron scattering and density-functional theory calculations to show that two antagonistic components define the magnetism in Mn-substituted SnTe, thereby limiting the effectiveness of dilute magnetic TIs. One component is strongly bound antiferromagnetic dimers that compete with ferromagnetic order. The other component consists of undimerized moments where ferromagnetic order develops via long-range interactions.

cond-mat.str-el↗

arXiv2023

Single crystal growth and characterization of antiferromagnetically ordering EuIn$_2$

We report the single crystal growth and characterization of EuIn$_2$, a magnetic topological semimetal candidate according to our density functional theory (DFT) calculations. We present results from electrical resistance, magnetization, Mössbauer spectroscopy, and X-ray resonant magnetic scattering (XRMS) measurements. We observe three magnetic transitions at $T_{\text{N}1}\sim 14.2~$K, $T_{\text{N}2}\sim12.8~$K and $T_{\text{N}3}\sim 11~$K, signatures of which are consistently seen in anisotropic temperature dependent magnetic susceptibility and electrical resistance data. Mössbauer spectroscopy measurements on ground crystals suggest an incommensurate sinusoidally modulated magnetic structure below the transition at $T_{\text{N}1}\sim 14~$K, followed by the appearance of higher harmonics in the modulation on further cooling roughly below $T_{\text{N}2}\sim13~$K, before the moment distribution squaring up below the lowest transition around $T_{\text{N}3}\sim 11~$K. XRMS measurements showed the appearance of magnetic Bragg peaks below $T_{\text{N}1}\sim14~$K, with a propagation vector of $\bmτ$ $=(τ_h,\barτ_h,0)$, with $τ_h$varying with temperature, and showing a jump at $T_{\text{N}3}\sim11$~K. The temperature dependence of $τ_h$ between $\sim11$~K and $14$~K shows incommensurate values consistent with the Mössbauer data. XRMS data indicate that $τ_h$ remains incommensurate at low temperatures and locks into $τ_h=0.3443(1)$.

cond-mat.mtrl-sci↗

arXiv2022

Competing magnetic fluctuations and orders in a multiorbital model of doped SrCo$_2$As$_2$

We revisit the intriguing magnetic behavior of the paradigmatic itinerant frustrated magnet $\rm{Sr}\rm{Co}_2\rm{As}_2$, which shows strong and competing magnetic fluctuations yet does not develop long-range magnetic order. By calculating the static spin susceptibility $χ(\mathbf{q})$ within a realistic sixteen orbital Hubbard-Hund model, we determine the leading instability to be ferromagnetic (FM). We then explore the effect of doping and calculate the critical Hubbard interaction strength $U_c$ that is required for the development of magnetic order. We find that $U_c$ decreases under electron doping and with increasing Hund's coupling $J$, but increases rapidly under hole doping. This suggests that magnetic order could possibly emerge under electron doping but not under hole doping, which agrees with experimental findings. We map out the leading magnetic instability as a function of doping and Hund's coupling and find several antiferromagnetic phases in addition to FM. We also quantify the degree of itinerant frustration in the model and resolve the contributions of different orbitals to the magnetic susceptibility. Finally, we discuss the dynamic spin susceptibility, $χ(\mathbf{q}, ω)$, at finite frequencies, where we recover the anisotropy of the peaks at $\mathbf{Q}_π= (π, 0)$ and $(0, π)$ observed by inelastic neutron scattering that is associated with the phenomenon of itinerant magnetic frustration. By comparing results between theory and experiment, we conclude that the essential experimental features of doped SrCo$_2$As$_2$ are well captured by a Hubbard-Hund multiorbital model if one considers a small shift of the chemical potential towards hole doping.

cond-mat.str-el↗

arXiv2022

Role of Magnetic Defects and Defect-engineering of Magnetic Topological Insulators

Magnetic defects play an important, but poorly understood, role in magnetic topological insulators (TIs). For example, topological surface transport and bulk magnetic properties are controlled by magnetic defects in Bi$_2$Se$_3$-based dilute ferromagnetic (FM) TIs and MnBi$_2$Te$_4$ (MBT)-based antiferromagnetic (AFM) TIs. Despite its nascent ferromagnetism, our inelastic neutron scattering data show that a fraction of the Mn defects in Sb$_2$Te$_3$ form strong AFM dimer singlets within a quintuple block. The AFM superexchange coupling occurs via Mn-Te-Mn linear bonds and is identical to the AFM coupling between antisite defects and the FM Mn layer in MBT, establishing common interactions in the two materials classes. We also find that the FM correlations in (Sb$_{1-x}$Mn$_x$)$_2$Te$_3$ are likely driven by magnetic defects in adjacent quintuple blocks across the van der Waals gap. In addition to providing answers to long-standing questions about the evolution of FM order in dilute TI, these results also show that the evolution of global magnetic order from AFM to FM in Sb-substituted MBT is controlled by defect engineering of the intrablock and interblock coupling.

cond-mat.mtrl-sci↗

arXiv2021

Defect-driven ferrimagnetism and hidden magnetization in MnBi$_2$Te$_4$

MnBi$_2$Te$_4$ (MBT) materials are promising antiferromagnetic topological insulators where field driven ferromagnetism is predicted to cause a transition between axion insulator and Weyl semimetallic states. However, the presence of antiferromagnetic coupling between Mn/Bi antisite defects and the main Mn layer can reduce the low-field magnetization, and it has been shown that such defects are more prevalent in the structurally identical trivial magnetic insulator MnSb$_2$Te$_4$ (MST). We use high-field magnetization measurements to show that the magnetization of MBT and MST occur in stages and full saturation requires fields of~$\sim$~60 Tesla. As a consequence, the low-field magnetization plateau state in MBT, where many determinations of quantum anomalous Hall state are studied, actually consists of ferrimagnetic septuple blocks containing both a uniform and staggered magnetization component.

cond-mat.mtrl-sci↗

arXiv2020

Formation of short-range magnetic order and avoided ferromagnetic quantum criticality in pressurized LaCrGe$_3$

LaCrGe$_3$ has attracted attention as a paradigm example of the avoidance of ferromagnetic (FM) quantum criticality in an itinerant magnet. By combining thermodynamic, transport, x-ray and neutron scattering as well as $μ$SR measurements, we refined the temperature-pressure phase diagram of LaCrGe$_3$. We provide thermodynamic evidence (i) for the first-order character of the FM transition when it is suppressed to low temperatures and (ii) for the formation of new phases at high pressures. From our microscopic data, we infer that short-range FM ordered clusters exist in these high-pressure phases. These results suggest that LaCrGe$_3$ is a rare example, which fills the gap between the two extreme limits of avoided FM quantum criticality in clean and strongly disordered metals.

cond-mat.str-el↗

arXiv2020

Controlling Magnetic Order, Magnetic Anisotropy, and Band Topology in Semimetals ${\rm Sr(Mn_{0.9}Cu_{0.1})Sb_2}$ and ${\rm Sr(Mn_{0.9}Zn_{0.1})Sb_2}$

Neutron diffraction and magnetic susceptibility studies show that orthorhombic single-crystals of topological semimetals ${\rm Sr(Mn_{0.9}Cu_{0.1})Sb_2}$ and ${\rm Sr(Mn_{0.9}Zn_{0.1})Sb_2}$ undergo three dimensional C-type antiferromagnetic (AFM) ordering of the Mn$^{2+}$ moments at $T_N = 200\pm10$ and $210\pm12$ K, respectively, significantly lower than that of the parent SrMnSb$_2$ with $T_N=297 \pm 3$ K. Magnetization versus applied magnetic field (perpendicular to MnSb planes) below $T_N$ exhibits slightly modified de Haas van Alphen oscillations for the Zn-doped crystal as compared to that of the parent compound. By contrast, the Cu-doped system does not show de Haas van Alphen magnetic oscillations, suggesting that either Cu substitution for Mn changes the electronic structure of the parent compound substantially, or that the Cu sites are strong scatterers of carriers that significantly shorten their mean free path thus diminishing the oscillations. Density functional theory (DFT) calculations including spin-orbit coupling predict the C-type AFM state for the parent, Cu-, and Zn-doped systems and identify the $a$-axis (i.e., perpendicular to the Mn layer) as the easy magnetization direction in the parent and 12.5% of Cu or Zn substitutions. In contrast, 25% of Cu content changes the easy magnetization to the $b$-axis (i.e., within the Mn layer). We find that the incorporation of Cu and Zn in SrMnSb$_2$ tunes electronic bands near the Fermi level resulting in different band topology and semi-metallicity. The parent and Zn-doped systems have coexistence of electron and hole pockets with opened Dirac cone around the Y-point whereas the Cu-doped system has dominant hole pockets around the Fermi level with a distorted Dirac cone. The tunable electronic structure may point out possibilities of rationalizing the experimentally observed de Haas van Alphen magnetic oscillations.

cond-mat.mtrl-sci↗

arXiv2020

Spin Dynamics in the Antiferromagnetic Oxypnictides and Fluoropnictides: LaMnAsO, LaMnSbO, and BaMnAsF

Inelastic neutron scattering (INS) from polycrystalline antiferromagnetic LaMnAsO, LaMnSbO, and BaMnAsF are analyzed using a $J_1-J_2-J_c$ Heisenberg model in the framework of the linear spin-wave theory. All three systems show clear evidence that the nearest- and next-nearest-neighbor interactions within the Mn square lattice layer ($J_1$ and $J_2$) are both antiferromagnetic (AFM). However, for all compounds studied the competing interactions have a ratio of $2J_2/J_1 < 1$, which favors the square lattice checkerboard AFM structure over the stripe AFM structure. The inter-plane coupling $J_c$ in all three systems is on the order of $\sim 3\times10^{-4}J_1$, rendering the magnetic properties of these systems with quasi-two-dimensional character. The substitution of Sb for As significantly lowers the in-plane exchange coupling, which is also reflected in the decrease of the N{é}el temperature, $T_{\rm N}$. Although BaMnAsF shares the MnAs sheets as LaMnAsO, their $J_1$ and $J_2$ values are substantially different. Using density functional theory, we calculate exchange parameters $J_{ij}$ to rationalize the differences among these systems.

cond-mat.str-el↗

arXiv2020

Manipulating of magnetism in the topological semimetal EuCd2As2

Magnetic Weyl semimetals are expected to have extraordinary physical properties such as a chiral anomaly and large anomalous Hall effects that may be useful for future, potential, spintronics applications. However, in most known host materials, multiple pairs of Weyl points prevent a clear manifestation of the intrinsic topological effects. Our recent density functional theory (DFT) calculations study suggest that EuCd$_{2}$As$_{2}$ can host Dirac fermions in an antiferromagnetically (AFM) ordered state or a single pair of Weyl fermions in a ferromagnetically (FM) ordered state. Unfortunately, previously synthesized crystals ordered antiferromagnetically with $T_{\textrm{N}}$\,$\simeq$\,9.5\,K. Here, we report the successful synthesis of single crystals of EuCd$_{2}$As$_{2}$ that order ferromagnetically (FM) or antiferromagnetically (AFM) depending on the level of band filling, thus allowing for the use of magnetism to tune the topological properties within the same host. We explored their physical properties via magnetization, electrical transport, heat capacity, and angle resolved photoemission spectroscopy (ARPES) measurements and conclude that EuCd$_{2}$As$_{2}$ is an excellent, tunable, system for exploring the interplay of magnetic ordering and topology.

cond-mat.mtrl-sci↗

arXiv2019

Hole Doping and Antiferromagnetic Correlations above the N{é}el temperature of the Topological Semimetal (Sr$_{1-x}$K$_x$)MnSb$_2$

Neutron diffraction and magnetic susceptibility studies of orthorhombic single crystal {\Ksub} confirm the three dimensional (3D) C-type antiferromagnetic (AFM) ordering of the Mn$^{2+}$ moments at $T_{\rm N}=305 \pm 3$ K which is slightly higher than that of the parent SrMnSb$_2$ with $T_{\rm N}=297 \pm 3$ K. Susceptibility measurements of the K-doped and parent crystals above $T_{\rm N}$ are characteristic of 2D AFM systems. This is consistent with high temperature neutron diffraction of the parent compound that display persisting 2D AFM correlations well above $T_{\rm N}$ to at least $\sim 560$ K with no evidence of a ferromagnetic phase. Analysis of the de Haas van Alphen magnetic oscillations of the K-doped crystal is consistent with hole doping.

cond-mat.str-el↗

arXiv2019

Two dimensional ordering and collective magnetic excitations in the dilute ferromagnetic topological insulator (Bi$_{0.95}$Mn$_{0.05}$)$_{2}$Te$_{3}$

Employing elastic and inelastic neutron scattering (INS) techniques, we report on detailed microscopic properties of the ferromagnetism in he magnetic topological insulator (Bi$_{0.95}$Mn$_{0.05}$)$_{2}$Te$_{3}$. Neutron diffraction of polycrystalline samples show the ferromagnetic (FM) ordering is long-range within the basal plane, and mainly 2D in character with short-range correlations between layers below $T_{\mathrm{C}} \approx 13$ K. Despite the random distribution of the dliute Mn atoms, we find that the 2D-like magnetic peaks are commensurate with the chemical structure, and the absence of (00L) magnetic peaks denote that the Mn$^{2+}$ magnetic moments are normal to the basal planes. Surprisingly, we observed collective magnetic excitations, in this dilute magnetic system. Despite the dilute nature, the excitations are typical of quasi-2D FM systems, albeit are severely broadened at short wavelengths, likely due to the random spatial distribution of Mn atoms in the Bi planes. Detailed analysis of the INS provide energy scales of the exchange couplings and the single ion anisotropy.

cond-mat.mtrl-sci↗

arXiv2019

Crystal growth, microstructure and physical properties of SrMnSb$_2$

We report on the crystal and magnetic structures, magnetic, and transport properties of SrMnSb$_2$ single crystals grown by the self-flux method. Magnetic susceptibility measurements reveal an antiferromagnetic (AFM) transition at $T_{\rm N} = 295(3)$ K. Above $T_{\rm N}$, the susceptibility slightly increases and forms a broad peak at $T \sim 420$ K, which is a typical feature of two-dimensional magnetic systems. Neutron diffraction measurements on single crystals confirm the previously reported C-type AFM structure below $T_{\rm N}$. Both de Haas-van Alphen (dHvA) and Shubnikov-de Haas (SdH) effects are observed in SrMnSb$_2$ single crystals. Analysis of the oscillatory component by a Fourier transform shows that the prominent frequencies obtained by the two different techniques are practically the same within error regardless of sample size or saturated magnetic moment. Transmission electron microscopy (TEM) reveals the existence of stacking faults in the crystals, which result from a horizontal shift of Sb atomic layers suggesting possible ordering of Sb vacancies in the crystals. Increase of temperature in susceptibility measurements leads to the formation of a strong peak at $T \sim {570}$ K that upon cooling under magnetic field the susceptibility shows a ferromagnetic transition at $T_{\rm C} \sim 580$ K. Neutron powder diffraction on crushed single-crystals does not support an FM phase above $T_{\rm N}$. Furthermore, X-ray magnetic circular dichroism (XMCD) measurements of a single crystal at the $L_{2,3}$ edge of Mn shows a signal due to induced canting of AFM moments by the applied magnetic field. All evidence strongly suggests that a chemical transformation at the surface of single crystals occurs above 500 K concurrently producing a minute amount of ferromagnetic impurity phase.

cond-mat.mtrl-sci↗

arXiv2019

A Single Pair of Weyl Fermions in Half-metallic EuCd2As2 Semimetal

An ideal Weyl semimetal with a single pair of Weyl points (WPs) may be generated by splitting a single Dirac point (DP) through the breaking of time-reversal symmetry by magnetic order. However, most known Dirac semimetals possess a pair of DPs along an axis that is protected by crystalline symmetry. Here, we demonstrate that a single pair of WPs may also be generated from a pair of DPs. Using first-principles band structure calculations, we show that inducing ferromagnetism in the AFM Dirac semimetal EuCd2As2 generates a single pair of WPs due to its half-metallic nature. Analysis with a low-energy effective Hamiltonian shows that this ideal Weyl semimetal is obtained in EuCd2As2 because the DPs are very close to the zone center and the ferromagnetic exchange splitting is large enough to push one pair of WPs to merge and annihilate at Gamma while the other pair survives. Furthermore, we predict that alloying with Ba at the Eu site can stabilize the ferromagnetic configuration and generate a single pair of Weyl points without application of a magnetic field.

cond-mat.mtrl-sci↗