Showing 1–50 of 105 results for author: May, A F

Observation geometry for uncertainty-aware Hamiltonian inference and experimental design in quantum magnets

Authors: Roy Liu, Venugopal Ranganathan, David Dahlbom, Shizhou Xu, Tianyu Zhang, Yuan Ni, Daniel M. Pajerowski, Garrett Granroth, Thomas Strohmer, Matthew B. Stone, Andrew F. May, Mark D. Lumsden, Joshua J. Turner, Yongqiang Cheng, Zhantao Chen

Abstract: Determining microscopic interactions from spectroscopic and scattering measurements is central to understanding quantum materials, yet it often remains unclear which interactions can be reliably revealed by the available experimental data and how additional experimental modalities should be designed to resolve the remaining ambiguities. Here we present an artificial intelligence-enabled framework… ▽ More Determining microscopic interactions from spectroscopic and scattering measurements is central to understanding quantum materials, yet it often remains unclear which interactions can be reliably revealed by the available experimental data and how additional experimental modalities should be designed to resolve the remaining ambiguities. Here we present an artificial intelligence-enabled framework for uncertainty-aware Hamiltonian inference and adaptive experimental design. By combining Hamiltonian-conditioned neural surrogates with Bayesian inference and observation geometry, the framework characterizes how measurements constrain Hamiltonian parameter space, quantifies the identifiability of microscopic interactions, and propagates posterior uncertainty directly in the physical Hamiltonian parameter space rather than an abstract learned representation. Using multimodal powder and single-crystal inelastic neutron scattering measurements of the quantum magnet NiPS$_{3}$, we demonstrate physically interpretable Hamiltonian inference, modality-aware uncertainty quantification, and adaptive experimental design. The framework provides a general strategy for uncertainty-aware microscopic characterization and multimodal experimental design across quantum materials. △ Less

Submitted 10 August, 2026; originally announced August 2026.

Nonresonant optomechanical control of structural phases

Authors: Jiaojian Shi, Yijing Huang, Christian Heide, Elias Hilderbrand, Carl Friedrich Schon, Jan Kottgen, Matthias Wuttig, Burak Guzelturk, Isabel Sedwick, Yukun Li, Haowei Xu, Yuejun Shen, Pooja Donthi Reddy, Viktoryia Shautsova, Mohammad Taghinejad, Duan Luo, Mark L. Brongersma, Kunal Mukherjee, Yuki Kobayashi, Andrew F. May, Eamonn Hughes, Mariano Trigo, David A. Reis, Ju Li, Jian Zhou , et al. (2 additional authors not shown)

Abstract: Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases giv… ▽ More Optical tweezers demonstrate how light can exert forces to trap, repel, and manipulate microscopic particles without absorption. Recent theory has suggested that such forces can extend beyond particle manipulation to drive structural phase transitions in solids. Here we apply this optomechanical principle to tin selenide (SnSe), a material where proximity to several different structural phases gives rise to its high thermoelectric figure of merit and makes it a candidate for a switchable topological crystalline insulator. Whereas the force for standard optical tweezers arises from a gradient in the intensity of a light field, the optomechanical force is mediated by a gradient in the dielectric constant as a function of phonon coordinate. Unlike conventional methods that rely on resonant excitation and absorption through the imaginary part of the dielectric function, this approach operates dispersively through the real part and can be directly driven by Raman processes, enabling selective transitions with reduced energy cost and ultrafast response. Using time-domain Raman scattering, we show that above a critical mid-infrared field strength the $A_g$ Raman modes disappear abruptly without softening, signaling the formation of a new structural phase. This phase, distinct from those induced by heating or carrier excitation, exhibits large-amplitude and long-lived modulations in its optical response. Complementing this observation, we show also evidence for an equivalent DC-field-driven structural phase transformation to a higher symmetry phase, as observed by atom probe tomography. Our study demonstrates the concept of nonresonant optomechanical phase control and defines novel opportunities for synthesizing hidden structural phases with unique functional properties. △ Less

Submitted 9 August, 2026; originally announced August 2026.

Comments: 5 figures

Frustration induced dimensional reduction and coexistence of long and short-range magnetic order in NdCl$_{3}$

Authors: Eli Zoghlin, Matthew B. Stone, Vasile O. Garlea, Matthias D. Frontzek, Andrew D. Christianson, Andrew F. May

Abstract: The phenomenon of frustration greatly enriches the accessible physics of quantum magnets. With this in mind we study the magnetism of NdCl$_{3}$ using a combination of bulk properties measurements and neutron scattering techniques. The low-temperature heat capacity reveals two magnetic transitions at $T_{N1}$ = 270 mK and $T_{N2}$ = 180 mK. However, much of the magnetic entropy is released above… ▽ More The phenomenon of frustration greatly enriches the accessible physics of quantum magnets. With this in mind we study the magnetism of NdCl$_{3}$ using a combination of bulk properties measurements and neutron scattering techniques. The low-temperature heat capacity reveals two magnetic transitions at $T_{N1}$ = 270 mK and $T_{N2}$ = 180 mK. However, much of the magnetic entropy is released above $T_{N1}$, manifesting as a broad peak centered at $T^{*} \approx$ 450 mK. Single crystal elastic neutron scattering reveals highly anisotropic magnetic diffuse scattering above $T_{N2}$, confirming that quasi-one-dimensional, short-range, antiferromagnetic order is the origin of the broad peak in the heat capacity. Magnetic Bragg peaks characterized by a $\vec{k}$ = ($0$ $0$ $\frac{1}{2}$) propagation vector emerge below $T_{N1}$. Interestingly, the magnetic diffuse scattering persists for $T_{N2} < T < T_{N1}$, indicating a regime of coexisting short and long-range order. The magnetic Bragg peaks exhibit an additional increase in intensity below $T_{N2}$ with no change in $\vec{k}$. Concomitantly, the diffuse scattering disappears indicating the attainment of full long-range order. While the precise nature of the ordered magnetic ground state remains unresolved, the observed magnetic scattering indicates predominate $c$-axis moments with a small $ab$-plane component. We propose that the quasi-one-dimensional behavior and the coexistence of short and long-range order are driven by frustration of anisotropic exchange interactions. △ Less

Submitted 20 July, 2026; originally announced July 2026.

Comments: 15 pages, 6 figures, 2+A1 tables, submitted to Physical Review B

Anisotropic magnetism and Kondo-lattice behavior in the frustrated antiferromagnet Ce3MgBi5

Authors: Karolina Gornicka, Brenden R. Ortiz, Matthew S. Cook, Heda Zhang, Andrew D. Christianson, Andrew F. May

Abstract: We report the synthesis and physical characterization of single-crystalline Ce3MgBi5, a previously unexplored member of the Ce3MPn5 family. This compound crystallizes in the hexagonal P63/mcm structure, featuring an anisotropic Ce sublattice composed of zig-zag chains along the c axis and a distorted kagome-like network in the basal plane. Magnetization measurements reveal antiferromagnetic order… ▽ More We report the synthesis and physical characterization of single-crystalline Ce3MgBi5, a previously unexplored member of the Ce3MPn5 family. This compound crystallizes in the hexagonal P63/mcm structure, featuring an anisotropic Ce sublattice composed of zig-zag chains along the c axis and a distorted kagome-like network in the basal plane. Magnetization measurements reveal antiferromagnetic order below TN approximately 4.2 K, accompanied by strong magnetic anisotropy and multiple field-induced metamagnetic transitions for fields applied perpendicular to [001], leading to a dome-shaped H-T phase diagram. Electrical transport exhibits characteristic signatures of a Ce-based Kondo lattice, including broad resistivity maxima and pronounced field-dependent anomalies in the magnetoresistance and Hall response that track the magnetic phase boundaries. Specific-heat measurements confirm the magnetic transition and show that the full R ln 2 entropy expected for a Ce3+ Kramers doublet is recovered by 20 K, indicating an extended temperature range of magnetic fluctuations consistent with Kondo correlations. Our results establish Ce3MgBi5 as a platform within the Ce3MPn5 family for exploring the interplay of geometric frustration, magnetic anisotropy, and Kondo-lattice physics under applied magnetic fields. △ Less

Submitted 27 May, 2026; originally announced May 2026.

Journal ref: Phys. Rev. Materials 10, 054413 (2026)

Magnetism of single crystalline breathing pyrochlore spinel AgInCr4S8

Authors: Andrew F. May, Christopher M. Pasco, V. O. Garlea, Karolina Gornicka, Matthias D. Frontzek, Xiaoping Wang, Pyeongjae Park, Andrew D. Christianson

Abstract: 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, sp… ▽ More 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. △ Less

Submitted 20 May, 2026; originally announced May 2026.

Journal ref: Physical Review MATERIALS 10, 054410 (2026)

Magnetic Imaging of Macroscopic Spin Chirality Flipping

Authors: H. Miao, G. Fabbris, J. Bouaziz, W. R. Meier, P. Mercado Lozano, Y. Choi, J. Strempfer, D. Haskel, S. Blügel, M. Cook, M. Brahlek, H. N. Lee, A. D. Christianson, A. F. May, S. Okamoto

Abstract: Chirality is a fundamental organizing principle of correlated and topological states. In quantum magnets, chirality arises from the geometric twisting of spins and serves as an emergent source of Berry curvature and quantum metrics. Although external fields can reversibly tune the spin chirality, understanding how spontaneous reversal occurs on macroscopic length scale remains an unresolved challe… ▽ More Chirality is a fundamental organizing principle of correlated and topological states. In quantum magnets, chirality arises from the geometric twisting of spins and serves as an emergent source of Berry curvature and quantum metrics. Although external fields can reversibly tune the spin chirality, understanding how spontaneous reversal occurs on macroscopic length scale remains an unresolved challenge. In this letter, we use resonant magnetic x-ray scattering with 2.5-micron spatial resolution to image intertwined spin, charge, and lattice orders of the correlated topological magnet EuAl4. We uncover a macroscopic chirality flipping transition and a remarkable chiral memory effect. The chiral magnetic domain tracks the landscape of the underlying charge density wave, implicating emergent chiral magnetic interactions arising from competing chiral and nematic lattice fields. Our results reveal the fundamental significance of magnetoelastic coupling in stabilizing homochiral and topological magnetic states. △ Less

Submitted 16 March, 2026; originally announced March 2026.

Dichotomy of flat bands in the van der Waals ferromagnet Fe$_5$GeTe$_2$

Authors: Han Wu, Jianwei Huang, Chaowei Hu, Lei Chen, Yiqing Hao, Yue Shi, Paul Malinowski, Yucheng Guo, Bo Gyu Jang, Jian-Xin Zhu, Andrew F. May, Siqi Wang, Xiang Chen, Yaofeng Xie, Bin Gao, Yichen Zhang, Ziqin Yue, Zheng Ren, Makoto Hashimoto, Donghui Lu, Alexei Fedorov, Sung-Kwan Mo, Junichiro Kono, Yu He, Robert J. Birgeneau , et al. (6 additional authors not shown)

Abstract: Quantum materials with bands of narrow bandwidth near the Fermi level represent a promising platform for exploring a diverse range of fascinating physical phenomena, as the high density of states within the small energy window often enables the emergence of many-body physics. On one hand, flat bands can arise from strong Coulomb interactions that localize atomic orbitals. On the other hand, quantu… ▽ More Quantum materials with bands of narrow bandwidth near the Fermi level represent a promising platform for exploring a diverse range of fascinating physical phenomena, as the high density of states within the small energy window often enables the emergence of many-body physics. On one hand, flat bands can arise from strong Coulomb interactions that localize atomic orbitals. On the other hand, quantum destructive interference can quench the electronic kinetic energy. Although both have a narrow bandwidth, the two types of flat bands should exhibit very distinct spectral properties arising from their distinctive origins. So far, the two types of flat bands have only been realized in very different material settings and chemical environments, preventing a direct comparison. Here, we report the observation of the two types of flat bands within the same material system--an above-room-temperature van der Waals ferromagnet, Fe$_{5-x}$GeTe$_2$, distinguishable by a switchable iron site order. The contrasting nature of the flat bands is also identified by the remarkably distinctive temperature-evolution of the spectral features, indicating that one arises from electron correlations in the Fe(1) site-disordered phase, while the other geometrical frustration in the Fe(1) site-ordered phase. Our results therefore provide a direct juxtaposition of the distinct formation mechanism of flat bands in quantum materials, and an avenue for understanding the distinctive roles flat bands play in the presence of magnetism, topology, and lattice geometrical frustration, utilizing sublattice ordering as a key control parameter. △ Less

Submitted 6 August, 2025; v1 submitted 4 August, 2025; originally announced August 2025.

Comments: The manuscript was submitted on June 12 2024

Journal ref: Phys. Rev. B 113, 125120 (2026)

Quantum Imaging of Ferromagnetic van der Waals Magnetic Domain Structures at Ambient Conditions

Authors: Bindu, Amandeep Singh, Amir Hen, Lukas Drago Cavar, Sebastian Maria Ulrich Schultheis, Shira Yochelis, Yossi Paltiel, Andrew F. May, Angela Wittmann, Mathias Klaui, Dmitry Budker, Hadar Steinberg, Nir Bar-Gill

Abstract: Recently discovered 2D van der Waals magnetic materials, and specifically Iron-Germanium-Telluride ($\rm Fe_{5}GeTe_{2}$), have attracted significant attention both from a fundamental perspective and for potential applications. Key open questions concern their domain structure and magnetic phase transition temperature as a function of sample thickness and external field, as well as implications fo… ▽ More Recently discovered 2D van der Waals magnetic materials, and specifically Iron-Germanium-Telluride ($\rm Fe_{5}GeTe_{2}$), have attracted significant attention both from a fundamental perspective and for potential applications. Key open questions concern their domain structure and magnetic phase transition temperature as a function of sample thickness and external field, as well as implications for integration into devices such as magnetic memories and logic. Here we address key questions using a nitrogen-vacancy center based quantum magnetic microscope, enabling direct imaging of the magnetization of $\rm Fe_{5}GeTe_{2}$ at sub-micron spatial resolution as a function of temperature, magnetic field, and thickness. We employ spatially resolved measures, including magnetization variance and cross-correlation, and find a significant spread in transition temperature yet with no clear dependence on thickness down to 15 nm. We also identify previously unknown stripe features in the optical as well as magnetic images, which we attribute to modulations of the constituting elements during crystal synthesis and subsequent oxidation. Our results suggest that the magnetic anisotropy in this material does not play a crucial role in their magnetic properties, leading to a magnetic phase transition of $\rm Fe_{5}GeTe_{2}$ which is largely thickness-independent down to 15 nm. Our findings could be significant in designing future spintronic devices, magnetic memories and logic with 2D van der Waals magnetic materials. △ Less

Submitted 27 July, 2025; originally announced July 2025.

Journal ref: ACS Applied Materials & Interfaces, 1944-8244 (2025)

From weakly interacting spinons to tightly bound triplons in the frustrated quantum spin-Peierls chain

Authors: Pyeongjae Park, Bo Xiao, Karolina Górnicka, Andrew F. May, Jiaqiang Yan, Ryoichi Kajimoto, Mitsutaka Nakamura, Matthew B. Stone, Gábor B. Halász, Andrew D. Christianson

Abstract: Fractionalized quasiparticles and their confinement into emergent bound states lie at the heart of modern quantum magnetism. While the evolution into magnonic bound states has been well characterized, experimental insight into the analogous transition to triplons remains limited. Here, using high-resolution neutron spectroscopy and state-of-the-art spin dynamics simulations, we uncover the transfo… ▽ More Fractionalized quasiparticles and their confinement into emergent bound states lie at the heart of modern quantum magnetism. While the evolution into magnonic bound states has been well characterized, experimental insight into the analogous transition to triplons remains limited. Here, using high-resolution neutron spectroscopy and state-of-the-art spin dynamics simulations, we uncover the transformation from weakly interacting spinons to tightly bound triplons in the spin-Peierls compound CuGeO3. Quantitative comparisons between the measured spectra and tensor network simulations reveal substantial next-nearest-neighbor frustration and weak external dimerization, placing the system deep within the spontaneously dimerized regime and near the exactly solvable Majumdar-Ghosh point. We further show an energy- and temperature-dependent evolution between two contrasting quasiparticle regimes: deconfined spinons with markedly suppressed interactions by frustration, and coherent triplonic bound states with no observable spinon degrees of freedom. Remarkably, triplon character persists into the two-particle regime, forming a structured two-triplon continuum with a spectral feature associated with a van Hove singularity at its lower boundary. These findings challenge the conventional view that robust triplons require strong external dimerization and demonstrate how the interplay between frustration and dimerization can reshape fractionalization and confinement. △ Less

Submitted 6 August, 2025; v1 submitted 25 July, 2025; originally announced July 2025.

Comments: 13 pages, 4 figures

Anisotropic magnetism of polymorphic ErAl3

Authors: Karolina Gornicka, Brenden R. Ortiz, Andrew D. Christianson, Andrew F. May

Abstract: ErAl$_3$ can form in either a trigonal ($α$) or cubic ($β$) polymorph and this paper investigates the physical properties of these polymorphs through characterizations of single crystals grown in an aluminum flux. We demonstrate that polymorph selection can be achieved based on the nominal composition of the crystal growth. Magnetic measurements confirm that both $β$-ErAl$_3$ and $α$-ErAl$_3$ orde… ▽ More ErAl$_3$ can form in either a trigonal ($α$) or cubic ($β$) polymorph and this paper investigates the physical properties of these polymorphs through characterizations of single crystals grown in an aluminum flux. We demonstrate that polymorph selection can be achieved based on the nominal composition of the crystal growth. Magnetic measurements confirm that both $β$-ErAl$_3$ and $α$-ErAl$_3$ order antiferromagnetically at low temperatures. $β$-ErAl$_3$ undergoes AFM ordering at a Néel temperature T$_N$ = 5.1 K, and the transition is suppressed continually with applied field. $α$-ErAl$_3$ displays more complex behavior, with successive magnetic transitions at T$_N$ = 5.7 K and T$_2$ = 4.6 K for zero field, where heat capacity and dilatometry measurements evidence that these transitions are second- and first-order, respectively. Under magnetic field, strong anisotropy is revealed in $α$-ErAl$_3$, with several step-like metamagnetic transitions observed below T$_2$ for H$\parallel$c. These transitions produce sequential magnetization plateaus near one-half of the apparent saturation magnetization. The electrical resistivity of $α$-ErAl$_3$ is strongly coupled to its magnetism. At $T$ = 2 K, we observe a positive magnetoresistance reaching 60\%, with distinct anomalies at the metamagnetic transitions. The results are summarized in $H$- $T$ phase diagrams that demonstrate complex magnetic behavior for $α$-ErAl$_3$, suggesting an important role of competing interactions in this metallic system that possesses characteristics of Ising physics. △ Less

Submitted 11 July, 2025; originally announced July 2025.

Journal ref: Phys. Rev. Materials 8, 114412 (2024)

Enhanced Neel temperature and unusual thermal expansion in flux-grown FeCrAs crystals

Authors: Michael A. McGuire, Matthew S. Cook, Brenden R. Ortiz, Jiaqiang Yan, Andrew F. May

Abstract: We report results from our experimental investigation of the distorted-kagome compound FeCrAs. For this work, we developed a procedure using tin metal as a flux to produce needlelike crystals. The crystals were characterized by single crystal x-ray diffraction as well as measurements of magnetization, electrical transport, and heat capacity. The physical behaviors are generally similar to publishe… ▽ More We report results from our experimental investigation of the distorted-kagome compound FeCrAs. For this work, we developed a procedure using tin metal as a flux to produce needlelike crystals. The crystals were characterized by single crystal x-ray diffraction as well as measurements of magnetization, electrical transport, and heat capacity. The physical behaviors are generally similar to published results on crystals grown from a stoichiometric melt with two notable exceptions. The Sommerfeld coefficient is found to be 18 mJ/K2/mol, a little more than half of the previously reported value, and the Neel temperature is found to be 150 K, about 25K higher than in previous reports. The reason for these discrepancies are uncertain, but they may be related to differences in stoichiometry or disorder; it is expected that the Cr/Fe ratio has some variability in this compound. In addition, we find unusual thermal expansion behavior, with an anomaly at the Neel temperature and nearly temperature independent thermal expansion along the hexagonal c-axis above this transition. This suggests significant spin-lattice coupling, which may provide insight into non-metallic transport properties that have been associated with anomalous charge carrier scattering. △ Less

Submitted 27 August, 2025; v1 submitted 27 May, 2025; originally announced May 2025.

Short-range magnetic order and planar anisotropy in the topological ferrimagnet Mn3Si2Te6

Authors: Raju Baral, Andrew F. May, Stuart Calder

Abstract: Mn3Si2Te6 is a ferrimagnetic topological nodal-line semiconductor that exhibits unconventional colossal magnetoresitance (CMR) behavior, with short-range spin fluctuations being potentially intimately linked to the emergent properties. In this work, we determine the short range magnetic order and quantify the local magnetic anisotropy through total neutron scattering and polarized neutron powder d… ▽ More Mn3Si2Te6 is a ferrimagnetic topological nodal-line semiconductor that exhibits unconventional colossal magnetoresitance (CMR) behavior, with short-range spin fluctuations being potentially intimately linked to the emergent properties. In this work, we determine the short range magnetic order and quantify the local magnetic anisotropy through total neutron scattering and polarized neutron powder diffraction (pNPD) measurements on polycrystalline Mn3Si2Te6. The real space local and long range spin structure was determined through the application of magnetic pair distribution function (mPDF) analysis, with measurements from the low temperature ordered phase to the high temperature paramagnetic state. Short-range order over a frustrated trimer of three nearest neighbors was found to exist well above the long range ferrimagnetic transition. pNPD measurements in the spin polarized paramagnetic state were used to extract the local site susceptibility tensor of the Mn ions to quantify the magnetic anisotropy. Our combined mPDF and pNPD results provide quantitative information on the short-range order intrinsic to Mn3Si2Te6, showing strong in-plane anisotropy with the spins largely confined to the ab-plane in zero field and remain stable with increasing temperature through the long-range to short-range ordered transition. △ Less

Submitted 10 April, 2025; originally announced April 2025.

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

Authors: Pyeongjae Park, Qianli Ma, G. Sala, S. Calder, Douglas L. Abernathy, Matthew B. Stone, Andrew F. May, Andrew D. Christianson

Abstract: 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-… ▽ More 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. △ Less

Submitted 24 March, 2025; v1 submitted 12 March, 2025; originally announced March 2025.

Comments: 12 pages, 6 figures

Journal ref: Phys. Rev. B 111, 104430 (2025)

Magnetic excitations and absence of charge order in the van der Waals ferromagnet Fe$_{4.75}$GeTe$_2$

Authors: V. K. Bhartiya, T. Kim, J. Li, T. P. Darlington, D. J. Rizzo, Y. Gu., S. Fan, C. Nelson, J. W. Freeland, X. Xu, D. N. Basov, J. Pelliciari, A. F. May, C. Mazzoli, V. Bisogni

Abstract: Understanding the ground state of van der Waals (vdW) magnets is crucial for designing devices leveraging these platforms. Here, we investigate the magnetic excitations and charge order in Fe$_{4.75}$GeTe$_2$, a vdW ferromagnet with $\approx$ 315 K Curie temperature. Using Fe $L_3 - $edge resonant inelastic x-ray scattering, we observe a dual nature of magnetic excitations, comprising a coherent m… ▽ More Understanding the ground state of van der Waals (vdW) magnets is crucial for designing devices leveraging these platforms. Here, we investigate the magnetic excitations and charge order in Fe$_{4.75}$GeTe$_2$, a vdW ferromagnet with $\approx$ 315 K Curie temperature. Using Fe $L_3 - $edge resonant inelastic x-ray scattering, we observe a dual nature of magnetic excitations, comprising a coherent magnon and a broad non-dispersive continuum extending up to 150 meV, 50$\%$ higher than in Fe$_{2.72}$GeTe$_2$. The continuum intensity is sinusoidally modulated along the stacking direction $L$, with a period matching the inter-slab distance. Our results indicate that while the dual character of the magnetic excitations is generic to Fe-Ge-Te vdW magnets, Fe$_{4.75}$GeTe$_2$ exhibits a longer out-of-plane magnetic correlation length, suggesting enhanced 3D magnetic character. Furthermore, resonant x-ray diffraction reveals that previously reported $\pm$(1/3, 1/3, $L$) peaks originate from crystal structure rather than from charge order. △ Less

Submitted 23 July, 2025; v1 submitted 19 November, 2024; originally announced November 2024.

Comments: 17 pages, 3 figures, supplementary file

Journal ref: npj Quantum Mater. 10, 80 (2025)

Incommensurate Transverse Peierls Transition

Authors: F. Z. Yang, K. F. Luo, Weizhe Zhang, Xiaoyu Guo, W. R. Meier, H. Ni, H. X. Li, P. Mercado Lozano, G. Fabbris, A. H. Said, C. Nelson, T. T. Zhang, A. F. May, M. A. McGuire, R. Juneja, L. Lindsay, H. N. Lee, J. -M. Zuo, M. F. Chi, X. Dai, Liuyan Zhao, H. Miao

Abstract: In one-dimensional quantum materials, conducting electrons and the underlying lattices can undergo a spontaneous translational symmetry breaking, known as Peierls transition. For nearly a century, the Peierls transition has been understood within the paradigm of electron-electron interactions mediated by longitudinal acoustic phonons. This classical picture has recently been revised in topological… ▽ More In one-dimensional quantum materials, conducting electrons and the underlying lattices can undergo a spontaneous translational symmetry breaking, known as Peierls transition. For nearly a century, the Peierls transition has been understood within the paradigm of electron-electron interactions mediated by longitudinal acoustic phonons. This classical picture has recently been revised in topological semimetals, where transverse acoustic phonons can couple with conducting p-orbital electrons and give rise to an unconventional Fermi surface instability, dubbed the transverse Peierls transition (TPT). Most interestingly, the TPT induced lattice distortions can further break rotation or mirror/inversion symmetries, leading to nematic or chiral charge density waves (CDWs). Quantum materials that host the TPT, however, have not been experimentally established. Here, we report the experimental discovery of an incommensurate TPT in the tetragonal Dirac semimetal EuAl$_4$. Using inelastic x-ray scattering with meV resolution, we observe the complete softening of a transverse acoustic phonon at the CDW wavevector upon cooling, whereas the longitudinal acoustic phonon is nearly unchanged. Combining with first principles calculations, we show that the incommensurate CDW wavevector matches the calculated charge susceptibility peak and connects the nested Dirac bands with Al 3$p_{x}$ and 3$p_{y}$ orbitals. Supplemented by second harmonic generation measurements, we show that the CDW induced lattice distortions break all vertical and diagonal mirrors whereas the four-fold rotational symmetry is retained below the CDW transition. Our observations strongly suggest a chiral CDW in EuAl$_4$ and highlight the TPT as a new avenue for chiral quantum states. △ Less

Submitted 14 October, 2024; originally announced October 2024.

Comments: Supplementary materials are available upon request

Journal ref: Nature Communications 16:10401 (2025)

MnRhBi3: A Cleavable Antiferromagnetic Metal

Authors: Eleanor M. Clements, Dmitry Ovchinnikov, Parul R. Raghuvanshi, Valentino R. Cooper, Satoshi Okamoto, Andrew D. Christianson, Joseph A. M. Paddison, Brenden R. Ortiz, Stuart Calder, Andrew F. May, Xiaodong Xu, Jiaqiang Yan, Michael A. McGuire

Abstract: Cleavable metallic antiferromagnets may be of use for low-dissipation spintronic devices; however, few are currently known. Here we present orthorhombic MnRhBi3 as one such compound and present a thorough study of its physical properties. Exfoliation is demonstrated experimentally, and the cleavage energy and electronic structure are examined by density functional theory calculations. It is conclu… ▽ More Cleavable metallic antiferromagnets may be of use for low-dissipation spintronic devices; however, few are currently known. Here we present orthorhombic MnRhBi3 as one such compound and present a thorough study of its physical properties. Exfoliation is demonstrated experimentally, and the cleavage energy and electronic structure are examined by density functional theory calculations. It is concluded that MnRhBi3 is a van der Waals layered material that cleaves easily between neighboring Bi layers, and that the Bi atoms have lone pairs extending into the van der Waals gaps. A series of four phase transitions are observed below room temperature, and neutron diffraction shows that at least two of the transitions involve the formation of antiferromagnetic order. Anomalous thermal expansion points to a crystallographic phase transition and/or strong magnetoelastic coupling. This work reveals a complex phase evolution in MnRhBi3 and establishes this cleavable antiferromagnetic metal as an interesting material for studying the interplay of structure, magnetism, and transport in the bulk and ultrathin limits as well as the role of lone pair electrons in interface chemistry and proximity effects in van der Waals heterostructures. △ Less

Submitted 30 June, 2024; originally announced July 2024.

Spin Dynamics of the Centrosymmetric Skyrmion Material GdRu2Si2

Authors: Joseph A. M. Paddison, Juba Bouaziz, Andrew F. May, Qiang Zhang, Stuart Calder, Douglas Abernathy, Julie B. Staunton, Stefan Blügel, Andrew D. Christianson

Abstract: Magnetic skyrmion crystals are traditionally associated with non-centrosymmetric crystal structures; however, it has been demonstrated that skyrmion crystals can be stabilized by competing interactions in centrosymmetric crystals. To understand and optimize the physical responses associated with topologically-nontrivial skyrmion textures, it is important to quantify their magnetic interactions by… ▽ More Magnetic skyrmion crystals are traditionally associated with non-centrosymmetric crystal structures; however, it has been demonstrated that skyrmion crystals can be stabilized by competing interactions in centrosymmetric crystals. To understand and optimize the physical responses associated with topologically-nontrivial skyrmion textures, it is important to quantify their magnetic interactions by comparing theoretical predictions with spectroscopic data. Here, we present neutron diffraction and spectroscopy data on the centrosymmetric skyrmion material GdRu$_2$Si$_2$, and show that the key spectroscopic features can be explained by the magnetic interactions calculated using density-functional theory calculations. We further show that the recently-proposed 2-$\mathbf{q}$ "topological spin stripe" structure yields better agreement with our data than a 1-$\mathbf{q}$ helical structure, and identify how the magnetic structure evolves with temperature. △ Less

Submitted 6 June, 2024; originally announced June 2024.

Comments: 6 pages, 3 figures

Codimension-Two Spiral Spin-Liquid in the Effective Honeycomb-Lattice Compound Cs$_3$Fe$_2$Cl$_9$

Authors: Shang Gao, Chris Pasco, Otkur Omar, Qiang Zhang, Daniel M. Pajerowski, Feng Ye, Matthias Frontzek, Andrew F. May, Matthew B. Stone, Andrew D. Christianson

Abstract: A codimension-two spiral spin-liquid is a correlated paramagnetic state with one-dimensional ground state degeneracy hosted within a three-dimensional lattice. Here, via neutron scattering experiments and numerical simulations, we establish the existence of a codimension-two spiral spin-liquid in the effective honeycomb-lattice compound Cs$_3$Fe$_2$Cl$_9$, which demonstrates a novel path to spiral… ▽ More A codimension-two spiral spin-liquid is a correlated paramagnetic state with one-dimensional ground state degeneracy hosted within a three-dimensional lattice. Here, via neutron scattering experiments and numerical simulations, we establish the existence of a codimension-two spiral spin-liquid in the effective honeycomb-lattice compound Cs$_3$Fe$_2$Cl$_9$, which demonstrates a novel path to spiral spin-liquids by overcoming the long-standing impediment of weak further-neighbor interactions. In the long-range ordered regime, competing spiral and spin density wave orders emerge as a function of applied magnetic field, among which a possible order-by-disorder transition is identified. △ Less

Submitted 10 January, 2026; v1 submitted 29 May, 2024; originally announced May 2024.

Comments: 21 pages, 19 figures, improved analysis of the INS spectra

Journal ref: Phys. Rev. B 113, L140401 (2026)

Intricate magnetic landscape in antiferromagnetic kagome metal TbTi$_3$Bi$_4$ and interplay with Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (Ln: Tb-Lu) shurikagome metals

Authors: Brenden R. Ortiz, Heda Zhang, Karolina Gornicka, David S. Parker, German D. Samolyuk, Fazhi Yang, Hu Miao, Qiangsheng Lu, Robert G. Moore, Andrew F. May, Michael A. McGuire

Abstract: Here we present the discovery and characterization of the kagome metal TbTi$_3$Bi$_4$ in tandem with a new series of compounds, the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (Ln: Tb-Lu) shurikagome metals. We previously reported on the growth of the LnTi$_3$Bi$_4$ (Ln: La-Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$) family, a chemically diverse and exfoliable series of kagome metals with complex and highly anisotropic magne… ▽ More Here we present the discovery and characterization of the kagome metal TbTi$_3$Bi$_4$ in tandem with a new series of compounds, the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (Ln: Tb-Lu) shurikagome metals. We previously reported on the growth of the LnTi$_3$Bi$_4$ (Ln: La-Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$) family, a chemically diverse and exfoliable series of kagome metals with complex and highly anisotropic magnetism. However, unlike the La-Gd analogs, TbTi$_3$Bi$_4$ cannot be synthesized by our previous methodology due to phase competition with Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ (x$\sim$1.7-1.2). Here we discuss the phase competition between the LnTi$_3$Bi$_4$ and Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ families, helping to frame the difficulty in synthesizing LnTi$_3$Bi$_4$ compounds with small Ln species and providing a strategy to circumvent formation of Ln$_{2-x}$Ti$_{6+x}$Bi$_9$. Detailed characterization of the magnetic and electronic transport properties on single crystals of TbTi$_3$Bi$_4$ reveals a highly complex landscape of magnetic phases arising from an antiferromagnetic ground state. A series of metamagnetic transitions creates at least 5 unique magnetic phase pockets, including a 1/3 and 2/3 magnetization plateau. Further, the system exhibits an intimate connection between the magnetism and magnetotransport, exhibiting sharp switching from positive (+40%) to negative magnetoresistance (-50%). Like the LnTi$_3$Bi$_4$ kagome metals, the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ family exhibits quasi-2D networks of titanium and chains of rare-earth. We present the structures and some basic magnetic properties of the Ln$_{2-x}$Ti$_{6+x}$Bi$_9$ family alongside our characterization of the newly discovered TbTi$_3$Bi$_4$. △ Less

Submitted 15 July, 2024; v1 submitted 18 May, 2024; originally announced May 2024.

Quantum and classical spin dynamics across temperature scales in the S = 1/2 Heisenberg antiferromagnet

Authors: Pyeongjae Park, G. Sala, Daniel M. Pajerowski, Andrew F. May, James A. Kolopus, D. Dahlbom, Matthew B. Stone, Gábor B. Halász, Andrew D. Christianson

Abstract: Using the framework of semi-classical Landau-Lifshitz dynamics (LLD), we conduct a systematic investigation of the temperature-dependent spin dynamics in the S = 1/2 Heisenberg square-lattice antiferromagnet (SqAF). By performing inelastic neutron scattering measurements on Zn2VO(PO4)2 (ZVPO) and corresponding finite-temperature spin dynamics simulations based on LLD, we present a comprehensive an… ▽ More Using the framework of semi-classical Landau-Lifshitz dynamics (LLD), we conduct a systematic investigation of the temperature-dependent spin dynamics in the S = 1/2 Heisenberg square-lattice antiferromagnet (SqAF). By performing inelastic neutron scattering measurements on Zn2VO(PO4)2 (ZVPO) and corresponding finite-temperature spin dynamics simulations based on LLD, we present a comprehensive analysis that bridges quantum and classical spin dynamics over a broad temperature range. First, a remarkable agreement between experimental data and LLD simulations is found in the paramagnetic phase of ZVPO, demonstrating the capability of LLD in accurately determining the spin Hamiltonian of S = 1/2 systems and capturing the quantum-to-classical crossover of their spin dynamics. Second, by analyzing the discrepancies between the experimental data and the LLD simulations at lower temperatures, we determine the experimental temperature dependence of the quantum effects in the excitation spectrum of the S = 1/2 SqAF: the quantum renormalization factor for the magnon energies and the quantum continuum above the one-magnon bands. Notably, the emergence of each quantum effect is found to correlate with the formation of three-dimensional long-range order. This work demonstrates the utility of LLD in gaining experimental insights into the temperature-induced modifications of quantum spin dynamics and their convergence towards classical expectations at higher temperatures. This motivates further applications to more challenging quantum antiferromagnets dominated by stronger quantum fluctuations. △ Less

Submitted 19 August, 2024; v1 submitted 14 May, 2024; originally announced May 2024.

Comments: 8 pages, 4 figures, Supplemental Material can be found on the journal's website

Journal ref: Phys. Rev. Research 6, 033184 (2024)

Anomalous continuum scattering and higher-order van Hove singularity in the strongly anisotropic S = 1/2 triangular lattice antiferromagnet

Authors: Pyeongjae Park, E. A. Ghioldi, Andrew F. May, James A. Kolopus, Andrey A. Podlesnyak, Stuart Calder, Joseph A. M. Paddison, A. E. Trumper, L. O. Manuel, Cristian D. Batista, Matthew B. Stone, Gabor B. Halasz, Andrew D. Christianson

Abstract: The S = 1/2 triangular lattice antiferromagnet (TLAF) is a paradigmatic example of frustrated quantum magnetism. An ongoing challenge involves understanding the influence of exchange anisotropy on the collective behavior within such systems. Using inelastic neutron scattering (INS) and advanced calculation techniques, we have studied the low and high-temperature spin dynamics of Ba2La2CoTe2O12 (BL… ▽ More The S = 1/2 triangular lattice antiferromagnet (TLAF) is a paradigmatic example of frustrated quantum magnetism. An ongoing challenge involves understanding the influence of exchange anisotropy on the collective behavior within such systems. Using inelastic neutron scattering (INS) and advanced calculation techniques, we have studied the low and high-temperature spin dynamics of Ba2La2CoTe2O12 (BLCTO): a Co2+-based Jeff = 1/2 TLAF that exhibits 120° order below TN = 3.26 K. We determined the spin Hamiltonian by fitting the energy-resolved paramagnetic excitations measured at T > TN, revealing exceptionally strong easy-plane XXZ anisotropy. Below TN, the excitation spectrum exhibits a high energy continuum having a larger spectral weight than the single-magnon modes, suggesting a scenario characterized by a spinon confinement length that markedly exceeds the lattice spacing. We conjecture that this phenomenon arises from the proximity to a quantum melting point, even under strong easy-plane XXZ anisotropy. Finally, we highlight characteristic flat features in the excitation spectrum, which are connected to higher-order van Hove singularities in the magnon dispersion directly induced by easy-plane XXZ anisotropy. Our results provide a rare experimental insight into the nature of highly anisotropic S = 1/2 TLAFs between the Heisenberg and XY limits. △ Less

Submitted 23 August, 2024; v1 submitted 5 March, 2024; originally announced March 2024.

Comments: 5 figures, Supplementary Information can be found on the journal's website

Journal ref: Nature Communications 15, 7264 (2024)

Quantum magnetism in the frustrated square lattice oxyhalides YbBi2IO4 and YbBi2ClO4

Authors: Pyeongjae Park, G. Sala, Th. Proffen, Matthew B. Stone, Andrew D. Christianson, Andrew F. May

Abstract: Square-lattice systems offer a direct route for realizing 2D quantum magnetism with frustration induced by competing interactions. In this work, the square-lattice materials YbBi2IO4 and YbBi2ClO4 were investigated using a combination of magnetization and specific heat measurements on polycrystalline samples. Specific heat measurements provide evidence for long-range magnetic order below TN = 0.21… ▽ More Square-lattice systems offer a direct route for realizing 2D quantum magnetism with frustration induced by competing interactions. In this work, the square-lattice materials YbBi2IO4 and YbBi2ClO4 were investigated using a combination of magnetization and specific heat measurements on polycrystalline samples. Specific heat measurements provide evidence for long-range magnetic order below TN = 0.21 K (0.25 K) for YbBi2IO4 (YbBi2ClO4). On the other hand, a rather broad maximum is found in the temperature-dependent magnetic susceptibility, located at Tmax = 0.33 K (0.38 K) in YbBi2IO4 (YbBi2ClO4), consistent with the quasi-2D magnetism expected for the large separation between the magnetic layers. Estimation of the magnetic entropy supports the expected Kramers' doublet ground state for Yb3+ and the observed paramagnetic behavior is consistent with a well-isolated doublet. Roughly two-thirds of the entropy is consumed above TN, due to a combination of the quasi-2D behavior and magnetic frustration. The impact of frustration is examined from the viewpoint of a simplified J1-J2 square lattice model, which is frustrated for antiferromagnetic interactions. Specifically, a high-temperature series expansion analysis of the temperature-dependent specific heat and magnetization data yields J2/J1 = 0.30 (0.23) for YbBi2IO4 (YbBi2ClO4). This simplified analysis suggests strong frustration that should promote significant quantum fluctuations in these compounds, and thus motivates future work on the static and dynamic magnetic properties of these materials. △ Less

Submitted 10 January, 2024; originally announced January 2024.

Comments: 8 pages, 5 figures

Journal ref: Phys. Rev. B 109, 014426 (2024)

Revisiting spin ice physics in the ferromagnetic Ising pyrochlore Pr$_2$Sn$_2$O$_7$

Authors: Brenden R. Ortiz, Paul M. Sarte, Ganesh Pokharel, Miles J. Knudston, Steven J. Gomez Alvarado, Andrew F. May, Stuart Calder, Lucile Mangin-Thro, Andrew R. Wildes, Haidong Zhou, Gabriele Sala, Chris R. Wiebe, Stephen D. Wilson, Joseph A. M. Paddison, Adam A. Aczel

Abstract: Pyrochlore materials are characterized by their hallmark network of corner-sharing rare-earth tetrahedra, which can produce a wide array of complex magnetic ground states. Ferromagnetic Ising pyrochlores often obey the "two-in-two-out" spin ice rules, which can lead to a highly-degenerate spin structure. Large moment systems, such as Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, tend to host a classica… ▽ More Pyrochlore materials are characterized by their hallmark network of corner-sharing rare-earth tetrahedra, which can produce a wide array of complex magnetic ground states. Ferromagnetic Ising pyrochlores often obey the "two-in-two-out" spin ice rules, which can lead to a highly-degenerate spin structure. Large moment systems, such as Ho$_2$Ti$_2$O$_7$ and Dy$_2$Ti$_2$O$_7$, tend to host a classical spin ice state with low-temperature spin freezing and emergent magnetic monopoles. Systems with smaller effective moments, such as Pr$^{3+}$-based pyrochlores, have been proposed as excellent candidates for hosting a "quantum spin ice" characterized by entanglement and a slew of exotic quasiparticle excitations. However, experimental evidence for a quantum spin ice state has remained elusive. Here, we show that the low-temperature magnetic properties of Pr$_2$Sn$_2$O$_7$ satisfy several important criteria for continued consideration as a quantum spin ice. We find that Pr$_2$Sn$_2$O$_7$ exhibits a partially spin-frozen ground state with a large volume fraction of dynamic magnetism. Our comprehensive bulk characterization and neutron scattering measurements enable us to map out the magnetic field-temperature phase diagram, producing results consistent with expectations for a ferromagnetic Ising pyrochlore. We identify key hallmarks of spin ice physics, and show that the application of small magnetic fields ($μ_0 H_c \sim$0.75T) suppresses the spin ice state and induces a long-range ordered magnetic structure. Together, our work clarifies the current state of Pr$_2$Sn$_2$O$_7$ and encourages future studies aimed at exploring the potential for a quantum spin ice ground state in this system. △ Less

Submitted 24 October, 2023; originally announced October 2023.

Evolution of highly anisotropic magnetism in the titanium-based kagome metals LnTi$_3$Bi$_4$ (Ln: La...Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$)

Authors: Brenden R. Ortiz, Hu Miao, David S. Parker, Fazhi Yang, German D. Samolyuk, Eleanor M. Clements, Anil Rajapitamahuni, Turgut Yilmaz, Elio Vescovo, Jiaqiang Yan, Andrew F. May, Michael A. McGuire

Abstract: Here we present the family of titanium-based kagome metals of the form LnTi$_3$Bi$_4$ (Ln: La...Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$). Single crystal growth methods are presented alongside detailed magnetic and thermodynamic measurements. The orthorhombic (Fmmm) LnTi$_3$Bi$_4$ family of compounds exhibit slightly distorted titanium-based kagome nets interwoven with zig-zag lanthanide-based (Ln) chains.… ▽ More Here we present the family of titanium-based kagome metals of the form LnTi$_3$Bi$_4$ (Ln: La...Gd$^{3+}$, Eu$^{2+}$, Yb$^{2+}$). Single crystal growth methods are presented alongside detailed magnetic and thermodynamic measurements. The orthorhombic (Fmmm) LnTi$_3$Bi$_4$ family of compounds exhibit slightly distorted titanium-based kagome nets interwoven with zig-zag lanthanide-based (Ln) chains. Crystals are easily exfoliated parallel to the kagome sheets and angular resolved photoemission (ARPES) measurements highlight the intricacy of the electronic structure in these compounds, with Dirac points existing at the Fermi level. The magnetic properties and the associated anisotropy emerge from the quasi-1D zig-zag chains of Ln, and impart a wide array of magnetic ground states ranging from anisotropic ferromagnetism to complex antiferromagnetism with a cascade of metamagnetic transitions. Kagome metals continue to provide a rich direction for the exploration of magnetic, topologic, and highly correlated behavior. Our work here introduces the LnTi$_3$Bi$_4$ compounds to augment the continuously expanding suite of complex and interesting kagome materials. △ Less

Submitted 6 September, 2023; v1 submitted 30 August, 2023; originally announced August 2023.

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

Authors: Tao Hong, Imam Makhfudz, Xianglin Ke, Andrew F. May, Andrey A. Podlesnyak, Daniel Pajerowski, Barry Winn, Merce Deumal, Yasumasa Takano, Mark M. Turnbull

Abstract: 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 evide… ▽ More 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. △ Less

Submitted 16 February, 2024; v1 submitted 9 June, 2023; originally announced June 2023.

Comments: 4 figures in the main text and 9 figures in the Supplementary Material. Any comments are welcome

Exchange bias between van der Waals materials: tilted magnetic states and field-free spin-orbit-torque switching

Authors: Thow Min Jerald Cham, Reiley J. Dorrian, Xiyue S. Zhang, Avalon H. Dismukes, Daniel G. Chica, Andrew F. May, Xavier Roy, David A. Muller, Daniel C. Ralph, Yunqiu Kelly Luo

Abstract: Magnetic van der Waals heterostructures provide a unique platform to study magnetism and spintronics device concepts in the two-dimensional limit. Here, we report studies of exchange bias from the van der Waals antiferromagnet CrSBr acting on the van der Waals ferromagnet Fe3GeTe2 (FGT). The orientation of the exchange bias is along the in-plane easy axis of CrSBr, perpendicular to the out-of-plan… ▽ More Magnetic van der Waals heterostructures provide a unique platform to study magnetism and spintronics device concepts in the two-dimensional limit. Here, we report studies of exchange bias from the van der Waals antiferromagnet CrSBr acting on the van der Waals ferromagnet Fe3GeTe2 (FGT). The orientation of the exchange bias is along the in-plane easy axis of CrSBr, perpendicular to the out-of-plane anisotropy of the FGT, inducing a strongly tilted magnetic configuration in the FGT. Furthermore, the in-plane exchange bias provides sufficient symmetry breaking to allow deterministic spin-orbit torque switching of the FGT in CrSBr/FGT/Pt samples at zero applied magnetic field. A minimum thickness of the CrSBr greater than 10 nm is needed to provide a non-zero exchange bias at 30 K. △ Less

Submitted 3 June, 2023; originally announced June 2023.

Multiple Incommensurate Magnetic States in the Kagome Antiferromagnet Na2Mn3Cl8

Authors: Joseph A. M. Paddison, Li Yin, Keith M. Taddei, Malcolm J. Cochran, Stuart A. Calder, David S. Parker, Andrew F. May

Abstract: The kagome lattice can host exotic magnetic phases arising from frustrated and competing magnetic interactions. However, relatively few insulating kagome materials exhibit incommensurate magnetic ordering. Here, we present a study of the magnetic structures and interactions of antiferromagnetic Na$_2$Mn$_3$Cl$_8$ with an undistorted Mn$^{2+}$ kagome network. Using neutron-diffraction and bulk magn… ▽ More The kagome lattice can host exotic magnetic phases arising from frustrated and competing magnetic interactions. However, relatively few insulating kagome materials exhibit incommensurate magnetic ordering. Here, we present a study of the magnetic structures and interactions of antiferromagnetic Na$_2$Mn$_3$Cl$_8$ with an undistorted Mn$^{2+}$ kagome network. Using neutron-diffraction and bulk magnetic measurements, we show that Na$_2$Mn$_3$Cl$_8$ hosts two different incommensurate magnetic states, which develop at $T_{N1} = 1.6$ K and $T_{N2} = 0.6$ K. Magnetic Rietveld refinements indicate magnetic propagation vectors of the form $\mathbf{q} = (q_{x},q_{y},\frac{3}{2})$, and our neutron-diffraction data can be well described by cycloidal magnetic structures. By optimizing exchange parameters against magnetic diffuse-scattering data, we show that the spin Hamiltonian contains ferromagnetic nearest-neighbor and antiferromagnetic third-neighbor Heisenberg interactions, with a significant contribution from long-ranged dipolar coupling. This experimentally-determined interaction model is compared with density-functional-theory simulations. Using classical Monte Carlo simulations, we show that these competing interactions explain the experimental observation of multiple incommensurate magnetic phases and may stabilize multi-$\mathbf{q}$ states. Our results expand the known range of magnetic behavior on the kagome lattice. △ Less

Submitted 17 April, 2023; originally announced April 2023.

Comments: 13 pages, 8 figures

Stability of the novel interorbital-hopping mechanism for ferromagnetism in multi-orbital Hubbard models

Authors: Ling-Fang Lin, Yang Zhang, Gonzalo Alvarez, Michael A. McGuire, Andrew F. May, Adriana Moreo, Elbio Dagotto

Abstract: Recently, it was argued that a ferromagnetic (FM) insulating phase can be induced by a novel {\it interorbital} hopping mechanism. Here, we study the stability range of this novel FM phase under modifications in the crystal fields and electronic correlation strength, constructing a theoretical phase diagram. A plethora of states is unveiled, including the FM Mott insulator (MI), a FM orbital-selec… ▽ More Recently, it was argued that a ferromagnetic (FM) insulating phase can be induced by a novel {\it interorbital} hopping mechanism. Here, we study the stability range of this novel FM phase under modifications in the crystal fields and electronic correlation strength, constructing a theoretical phase diagram. A plethora of states is unveiled, including the FM Mott insulator (MI), a FM orbital-selective Mott phase (OSMP), several anferromagnetic (AFM) MI phases, an AFM metallic state, and a FM metal as well. Our most interesting result is that the FM regime, either in MI or OSMP forms, is shown to be stable in {\it large} portions of the phase diagram, at both intermediate and strong electronic correlations, respectively. Our results demonstrate via a detailed example that the recently proposed novel mechanism to stabilize FM insulators is not fragile but instead robust, and may enlarge substantially the relatively small family of known FM insulators. △ Less

Submitted 14 March, 2023; originally announced March 2023.

Comments: 10 pages, 5 figures

Stacking disorder and thermal transport properties of $α$-RuCl$_3$

Authors: Heda Zhang, Michael A McGuire, Andrew F May, Joy Chao, Qiang Zheng, Miaofang Chi, Brian C Sales, David G Mandrus, Stephen E Nagler, Hu Miao, Feng Ye, Jiaqiang Yan

Abstract: $α$-RuCl$_3… ▽ More $α$-RuCl$_3$, a well-known candidate material for Kitaev quantum spin liquid, is prone to stacking disorder due to the weak van der Waals bonding between the honeycomb layers. After a decade of intensive experimental and theoretical studies, the detailed correlation between stacking degree of freedom, structure transition, magnetic and thermal transport properties remains unresolved. In this work, we reveal the effects of a small amount of stacking disorder inherent even in high quality $α$-RuCl$_3$ crystals. This small amount of stacking disorder results in the variation of the magnetic ordering temperature, suppresses the structure transition and thermal conductivity. Crystals with minimal amount of stacking disorder have a T$_N>$7.4\,K and exhibit a well-defined structure transition around 140\,K upon cooling. For those with more stacking faults and a T$_N$ below 7\,K, the structure transition occurs well below 140\,K upon cooling and is incomplete, manifested by the diffuse streaks and the coexistence of both high temperature and low temperature phases down to the lowest measurement temperature. Both types of crystals exhibit oscillatory field dependent thermal conductivity and a plateau-like feature in thermal Hall resistivity in the field-induced quantum spin liquid state. However, $α$-RuCl$_3$ crystals with minimal amount of stacking disorder have a higher thermal conductivity that pushes the thermal Hall conductivity to be closer to the half-integer quantized value. These findings demonstrate a strong correlation between layer stacking, structure transition, magnetic and thermal transport properties, underscoring the importance of interlayer coupling in $α$-RuCl$_3$ despite the weak van der Waals bonding. △ Less

Submitted 5 December, 2023; v1 submitted 7 March, 2023; originally announced March 2023.

Journal ref: Phys. Rev. Materials 8, 014402 (2024)

Determination of nonthermal bonding origin of a novel photoexcited lattice instability in SnSe

Authors: Yijing Huang, Samuel Teitelbaum, Shan Yang, Gilberto De la Pe na, Takahiro Sato Matthieu Chollet, Diling Zhu, Jennifer L. Niedziela, Dipanshu Bansal, Andrew F. May, Aaron M. Lindenberg, Olivier Delaire, Mariano Trigo, David A. Reis

Abstract: Interatomic forces that bind materials are largely determined by an often complex interplay between the electronic band-structure and the atomic arrangements to form its equilibrium structure and dynamics. As these forces also determine the phonon dispersion, lattice dynamics measurements are often crucial tools for understanding how materials transform between different structures. This is the ca… ▽ More Interatomic forces that bind materials are largely determined by an often complex interplay between the electronic band-structure and the atomic arrangements to form its equilibrium structure and dynamics. As these forces also determine the phonon dispersion, lattice dynamics measurements are often crucial tools for understanding how materials transform between different structures. This is the case for the mono-chalcogenides which feature a number of lattice instabilities associated with their network of resonant bonds and a large tunability in their functional properties. SnSe hosts a novel lattice instability upon above-bandgap photoexcitation that is distinct from the distortions associated with its high temperature phase transition, demonstrating that photoexcitation can alter the interatomic forces significantly different than thermal excitation. Here we report decisive time-resolved X-ray scattering-based measurements of the nonequlibrium lattice dynamics in SnSe. By fitting interatomic force models to the excited-state dispersion, we determine this instability as being primarily due to changes in the fourth-nearest neighbor bonds that connect bilayers, with relatively little change to the intralayer resonant bonds. In addition to providing critical insight into the nonthermal bonding origin of the instability in SnSe, such measurements will be crucial for understanding and controlling materials properties under non-equilibrium conditions. △ Less

Submitted 21 January, 2023; originally announced January 2023.

Superconductivity by alloying the topological insulator SnBi2Te4

Authors: Michael A. McGuire, Heda Zhang, Andrew F. May, Satoshi Okamoto, Robert G. Moore, Xiaoping Wang, Clément Girod, Sean M. Thomas, Filip Ronning, Jiaqiang Yan

Abstract: Alloying indium into the topological insulator Sn1-xInxBi2Te4 induces bulk superconductivity with critical temperatures Tc up to 1.85 K and upper critical fields up to about 14 kOe. This is confirmed by electrical resistivity, heat capacity, and magnetic susceptibility measurements. The heat capacity shows a discontinuity at Tc and temperature dependence below Tc consistent with weak coupling BCS… ▽ More Alloying indium into the topological insulator Sn1-xInxBi2Te4 induces bulk superconductivity with critical temperatures Tc up to 1.85 K and upper critical fields up to about 14 kOe. This is confirmed by electrical resistivity, heat capacity, and magnetic susceptibility measurements. The heat capacity shows a discontinuity at Tc and temperature dependence below Tc consistent with weak coupling BCS theory, and suggests a superconducting gap near 0.25 meV. The superconductivity is type-II and the topological surface states have been verified by photoemission. A simple picture suggests analogies with the isostructural magnetic topological insulator MnBi2Te4, in which a natural heterostructure hosts complementary properties on different sublattices, and motivates new interest in this large family of compounds. The existence of both topological surface states and superconductivity in Sn1-xInxBi2Te4 identifies these materials as promising candidates for the study of topological superconductivity. △ Less

Submitted 15 December, 2022; originally announced December 2022.

Dipolar spin ice regime proximate to an all-in-all-out Néel ground state in the dipolar-octupolar pyrochlore Ce$_2$Sn$_2$O$_7$

Authors: D. R. Yahne, B. Placke, R. Schäfer, O. Benton, R. Moessner, M. Powell, J. W. Kolis, C. M. Pasco, A. F. May, M. D. Frontzek, E. M. Smith, B. D. Gaulin, S. Calder, K. A. Ross

Abstract: The dipolar-octupolar (DO) pyrochlores, R$_2$M$_2$O$_7$ (R = Ce, Sm, Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce$_2$Sn$_2$O$_7$, synthesized by hydrothermal techniques, present an o… ▽ More The dipolar-octupolar (DO) pyrochlores, R$_2$M$_2$O$_7$ (R = Ce, Sm, Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce$_2$Sn$_2$O$_7$, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce$_2$Sn$_2$O$_7$ using the near-neighbor $XYZ$ model Hamiltonian associated with DO pyrochlores. Utilizing quantum numerical linked cluster expansion fits to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples, we place Ce$_2$Sn$_2$O$_7$'s ground state within the ordered dipolar all-in-all-out (AIAO) Néel phase, with quantum Monte Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce$_2$Sn$_2$O$_7$ powders show a broad signal at low scattering wave vectors, reminiscent of a \textit{dipolar} spin ice, in striking contrast from previous powder neutron diffraction on samples grown from solid-state synthesis, which found diffuse scattering at high scattering wave vectors associated with magnetic {\it octupoles} and suggested an octupolar quantum spin ice state. We conclude that new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO Néel order. △ Less

Submitted 26 January, 2024; v1 submitted 28 November, 2022; originally announced November 2022.

Comments: 16 pages, 12 figures

Journal ref: D. R. Yahne et al., Phys. Rev. X 14, 011005 (2024)

Line-Graph Approach to Spiral Spin Liquids

Authors: Shang Gao, Ganesh Pokharel, Andrew F. May, Joseph A. M. Paddison, Chris Pasco, Yaohua Liu, Keith M. Taddei, Stuart Calder, David G. Mandrus, Matthew B. Stone, Andrew D. Christianson

Abstract: Competition among exchange interactions is able to induce novel spin correlations on a bipartite lattice without geometrical frustration. A prototype example is the spiral spin liquid, which is a correlated paramagnetic state characterized by sub-dimensional degenerate propagation vectors. Here, using spectral graph theory, we show that spiral spin liquids on a bipartite lattice can be approximate… ▽ More Competition among exchange interactions is able to induce novel spin correlations on a bipartite lattice without geometrical frustration. A prototype example is the spiral spin liquid, which is a correlated paramagnetic state characterized by sub-dimensional degenerate propagation vectors. Here, using spectral graph theory, we show that spiral spin liquids on a bipartite lattice can be approximated by a further-neighbor model on the corresponding line-graph lattice that is non-bipartite, thus broadening the space of candidate materials that may support the spiral spin liquid phases. As illustrations, we examine neutron scattering experiments performed on two spinel compounds, ZnCr$_2$Se$_4$ and CuInCr$_4$Se$_8$, to demonstrate the feasibility of this new approach and expose its possible limitations in experimental realizations. △ Less

Submitted 21 October, 2022; originally announced October 2022.

Comments: 20 pages, 18 figures

Journal ref: Phys. Rev. Lett. 129, 237202 (2022)

Nanometric modulations of the magnetic structure of the element Nd

Authors: H. Suriya Arachchige, L. M. DeBeer-Schmitt, L. L. Kish, Binod K. Rai, A. F. May, D. S. Parker, G. Pokharel, Wei Tian, D. G. Mandrus, M. Bleuel, Z. Islam, G. Fabbris, H. X. Li, S. Gao, H. Miao, S. M. Thomas, P. F. S. Rosa, J. D. Thompson, Shi-Zeng Lin, A. D. Christianson

Abstract: The rare earth neodymium arguably exhibits the most complex magnetic ordering and series of magnetic phase transitions of the elements. Here we report the results of small-angle neutron scattering (SANS) measurements as a function of temperature and applied magnetic field to study magnetic correlations on nanometer length scales in Nd. The SANS measurements reveal the presence of previously unrepo… ▽ More The rare earth neodymium arguably exhibits the most complex magnetic ordering and series of magnetic phase transitions of the elements. Here we report the results of small-angle neutron scattering (SANS) measurements as a function of temperature and applied magnetic field to study magnetic correlations on nanometer length scales in Nd. The SANS measurements reveal the presence of previously unreported modulation vectors characterizing the ordered spin configuration which exhibit changes in magnitude and direction that are phase dependent. Between 5.9 and 7.6 K the additional modulation vector has a magnitude $Q$ =0.12 Å$^{-1}$ and is primarily due to order of the Nd layers which contain a center of inversion. In this region of the phase diagram, the SANS measurements also identify a phase boundary at $\approx$1 T. An important feature of these modulation vectors is that they indicate the presence of nanometer length scale spin textures which are likely stabilized by frustrated Ruderman-Kittel-Kasuya-Yosida (RKKY) interactions rather than a Dzyaloshinskii-Moriya (DM) exchange interaction. △ Less

Submitted 6 July, 2022; originally announced July 2022.

Comments: 16 pages, 15 figures

Above-room-temperature ferromagnetism in ultrathin van der Waals magnet

Authors: Hang Chen, Shahidul Asif, Kapildeb Dolui, Yang Wang, Jeyson Tamara Isaza, V. M. L. Durga Prasad Goli, Matthew Whalen, Xinhao Wang, Zhijie Chen, Huiqin Zhang, Kai Liu, Deep Jariwala, M. Benjamin Jungfleisch, Chitraleema Chakraborty, Andrew F. May, Michael A. McGuire, Branislav K. Nikolic, John Q. Xiao, Mark J. H. Ku

Abstract: Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling ultrathin and highly tunable spintronic devices. To realize high quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temp… ▽ More Two-dimensional (2D) magnetic van der Waals materials provide a powerful platform for studying fundamental physics of low-dimensional magnetism, engineering novel magnetic phases, and enabling ultrathin and highly tunable spintronic devices. To realize high quality and practical devices for such applications, there is a critical need for robust 2D magnets with ordering temperatures above room temperature that can be created via exfoliation. Here the study of exfoliated flakes of cobalt substituted Fe5GeTe2 (CFGT) exhibiting magnetism above room temperature is reported. Via quantum magnetic imaging with nitrogen-vacancy centers in diamond, ferromagnetism at room temperature was observed in CFGT flakes as thin as 16 nm. This corresponds to one of the thinnest room-temperature 2D magnet flakes exfoliated from robust single crystals, reaching a thickness relevant to practical spintronic applications. The Curie temperature Tc of CFGT ranges from 310 K in the thinnest flake studied to 328 K in the bulk. To investigate the prospect of high-temperature monolayer ferromagnetism, Monte Carlo calculations were performed which predicted a high value of Tc ~270 K in CFGT monolayers. Pathways towards further enhancing monolayer Tc are discussed. These results support CFGT as a promising platform to realize high-quality room-temperature 2D magnet devices. △ Less

Submitted 14 June, 2022; originally announced June 2022.

Controllable emergent spatial spin modulation in Sr2IrO4 by in situ shear strain

Authors: S. Pandey, H. Zhang, J. Yang, A. F. May, J. Sanchez, Z. Liu, J. -H. Chu, J. W. Kim, P. J. Ryan, H. D. Zhou, J. Liu

Abstract: Symmetric anisotropic interaction can be ferromagnetic and antiferromagnetic at the same time but for different crystallographic axes. We show that inducing competition of anisotropic interactions of orthogonal irreducible representations represents a general route to obtain new exotic magnetic states. We demonstrate it here by observing the emergence of a continuously tunable 12-layer spatial spi… ▽ More Symmetric anisotropic interaction can be ferromagnetic and antiferromagnetic at the same time but for different crystallographic axes. We show that inducing competition of anisotropic interactions of orthogonal irreducible representations represents a general route to obtain new exotic magnetic states. We demonstrate it here by observing the emergence of a continuously tunable 12-layer spatial spin modulation when distorting the square lattice planes in the quasi-2D antiferromagnetic Sr2IrO4 under in situ shear strain. This translation-symmetry-breaking phase is a result of an unusual strain activated anisotropic interaction which is at the 4th order and competing with the inherent quadratic anisotropic interaction. Such a mechanism of competing anisotropy is distinct from that among the ferromagnetic, antiferromagnetic, and/or the Dzyaloshinskii-Moriya interactions, and it could be widely applicable and highly controllable in low dimensional magnets. △ Less

Submitted 19 April, 2022; originally announced April 2022.

Gaps in Topological Magnon Spectra: Intrinsic vs. Extrinsic Effects

Authors: Seung-Hwan Do, Joseph A. M. Paddison, Gabriele Sala, Travis J. Williams, Koji Kaneko, Keitaro Kuwahara, A. F. May, Jiaqiang Yan, Michael A. McGuire, Matthew B. Stone, Mark D. Lumsden, Andrew D. Christianson

Abstract: For topological magnon spectra, determining and explaining the presence of a gap at a magnon crossing point is a key to characterize the topological properties of the system. An inelastic neutron scattering study of a single crystal is a powerful experimental technique that is widely employed to probe the magnetic excitation spectra of topological materials. Here, we show that when the scattering… ▽ More For topological magnon spectra, determining and explaining the presence of a gap at a magnon crossing point is a key to characterize the topological properties of the system. An inelastic neutron scattering study of a single crystal is a powerful experimental technique that is widely employed to probe the magnetic excitation spectra of topological materials. Here, we show that when the scattering intensity rapidly disperses in the vicinity of a crossing point, such as a Dirac point, the apparent topological gap size is extremely sensitive to experimental conditions including sample mosaic, resolution, and momentum integration range. We demonstrate these effects using comprehensive neutron-scattering measurements of CrCl$_3$. Our measurements confirm the gapless nature of the Dirac magnon in CrCl$_3$, but also reveal an artificial, i.e. extrinsic, magnon gap unless the momentum integration range is carefully controlled. Our study provides an explanation of the apparent discrepancies between spectroscopic and first-principles estimates of Dirac magnon gap sizes, and provides guidelines for accurate spectroscopic measurement of topological magnon gaps. △ Less

Submitted 7 April, 2022; originally announced April 2022.

Comments: 6 pages and 4 figures

Thermodynamic insights into the intricate magnetic phase diagram of EuAl$_{4}$

Authors: William R. Meier, James R. Torres, Raphael P. Hermann, Jiyong Zhao, Barbara Lavina, Brian C. Sales, Andrew F. May

Abstract: The tetragonal intermetallic compound EuAl$_{4}$ hosts an exciting variety of low temperature phases. In addition to a charge density wave below 140 K, four ordered magnetic phases are observed below 15.4 K. Recently, a skyrmion phase was proposed based on Hall effect measurements under a $c$-axis magnetic field. We present a detailed investigation of the phase transitions in EuAl$_{4}$ under $c$-… ▽ More The tetragonal intermetallic compound EuAl$_{4}$ hosts an exciting variety of low temperature phases. In addition to a charge density wave below 140 K, four ordered magnetic phases are observed below 15.4 K. Recently, a skyrmion phase was proposed based on Hall effect measurements under a $c$-axis magnetic field. We present a detailed investigation of the phase transitions in EuAl$_{4}$ under $c$-axis magnetic field. Our dilatometry, heat capacity, DC magnetometry, AC magnetic susceptibility, and resonant ultrasound spectroscopy measurements reveal three magnetic phase transitions not previously reported. We discuss what our results reveal about the character of the magnetic phases. Our first key result is a detailed $H \parallel [001]$ magnetic phase diagram mapping the seven phases we observe. Second, we identify a new high-field phase, phase VII, which directly corresponds to the region were skyrmions have been suggested. Our results provide guidance for future studies exploring the complex magnetic interactions and spin structures in EuAl$_{4}$. △ Less

Submitted 5 April, 2022; originally announced April 2022.

Comments: 20 pages, 15 figures

Magnetic Interactions of the Centrosymmetric Skyrmion Material Gd2PdSi3

Authors: Joseph A. M. Paddison, Binod K. Rai, Andrew F. May, Stuart A. Calder, Matthew B. Stone, Matthias D. Frontzek, Andrew D. Christianson

Abstract: The experimental realization of magnetic skyrmions in centrosymmetric materials has been driven by theoretical understanding of how a delicate balance of anisotropy and frustration can stabilize topological spin structures in applied magnetic fields. Recently, the centrosymmetric material Gd$_{2}$PdSi$_{3}$ was shown to host a field-induced skyrmion phase, but the skyrmion stabilization mechanism… ▽ More The experimental realization of magnetic skyrmions in centrosymmetric materials has been driven by theoretical understanding of how a delicate balance of anisotropy and frustration can stabilize topological spin structures in applied magnetic fields. Recently, the centrosymmetric material Gd$_{2}$PdSi$_{3}$ was shown to host a field-induced skyrmion phase, but the skyrmion stabilization mechanism remains unclear. Here, we employ neutron-scattering measurements on an isotopically-enriched polycrystalline Gd$_{2}$PdSi$_{3}$ sample to quantify the interactions that drive skyrmion formation. Our analysis reveals spatially-extended interactions in triangular planes that are consistent with an RKKY mechanism, and large ferromagnetic inter-planar magnetic interactions that are modulated by the Pd/Si superstructure. The skyrmion phase emerges from a zero-field helical magnetic order with magnetic moments perpendicular to the magnetic propagation vector, indicating that the magnetic dipolar interaction plays a significant role. Our experimental results establish an interaction space that can promote skyrmion formation, facilitating identification and design of centrosymmetric skyrmion materials. △ Less

Submitted 28 February, 2022; originally announced March 2022.

Comments: 5 pages, 5 figures

Flat-Band Itinerant Antiferromagnetism in the Kagome Metal CoSn1-xInx

Authors: B. C. Sales, W. R. Meier, D. S. Parker, L. Yin, J. Q. Yan, A. F. May, S. Calder, A. A. Aczel, Q. Zhang, H. Li, T. Yilmaz, E. Vescovo, H. Miao, R. P. Hermann, M. A. McGuire

Abstract: Destructive interference of electron hopping on the frustrated kagome lattice generates Dirac nodes, saddle points, and flat bands in the electronic structure. The latter provides the narrow bands and a peak in the density of states that can generate correlated electron behavior when the Fermi level lies within them. In the kagome metal CoSn, this alignment is not realized, and the compound is a P… ▽ More Destructive interference of electron hopping on the frustrated kagome lattice generates Dirac nodes, saddle points, and flat bands in the electronic structure. The latter provides the narrow bands and a peak in the density of states that can generate correlated electron behavior when the Fermi level lies within them. In the kagome metal CoSn, this alignment is not realized, and the compound is a Pauli paramagnet. Here we show that replacing part of the tin with indium (CoSn1-xInx) moves the Fermi energy into the flat band region, with support from band structure calculations, heat capacity measurements, and angle resolved photoemission spectroscopy. The associated instability results in the emergence of itinerant antiferromagnetism with a Neel temperature up to 30K. Long range magnetic order is confirmed by neutron diffraction measurements, which indicate an ordered magnetic moment of 0.1-0.2 Bohr magnetons per Co (for x = 0.4). Thus, CoSn1-xInx provides a rare example of an itinerant antiferromagnet with a small ordered moment. This work provides clear evidence that flat bands arising from frustrated lattices in bulk crystals represent a viable route to new physics, evidenced here by the emergence of magnetic order upon introducing a non-magnetic dopant into a non-magnetic kagome metal. △ Less

Submitted 28 January, 2022; originally announced January 2022.

Journal ref: Chemistry of Materials 34, 7069 (2024)

Antiferromagnetic fluctuations and orbital-selective Mott transition in the van der Waals ferromagnet Fe3-xGeTe2

Authors: Xiaojian Bai, Frank Lechermann, Yaohua Liu, Yongqiang Cheng, Alexander I. Kolesnikov, Feng Ye, Travis J. Williams, Songxue Chi, Tao Hong, Garrett E. Granroth, Andrew F. May, Stuart Calder

Abstract: Fe3-xGeTe2 is a layered magnetic van der Waals material of interest for both fundamental and applied research. Despite the observation of intriguing physical properties, open questions exist even on the basic features related to magnetism: is it a simple ferromagnet or are there antiferromagnetic regimes and are the moments local or itinerant. Here, we demonstrate that antiferromagnetic spin fluct… ▽ More Fe3-xGeTe2 is a layered magnetic van der Waals material of interest for both fundamental and applied research. Despite the observation of intriguing physical properties, open questions exist even on the basic features related to magnetism: is it a simple ferromagnet or are there antiferromagnetic regimes and are the moments local or itinerant. Here, we demonstrate that antiferromagnetic spin fluctuations coexist with the ferromagnetism through comprehensive elastic and inelastic neutron scattering and thermodynamic measurements. Our realistic dynamical mean-field theory calculations reveal that the competing magnetic fluctuations are driven by an orbital selective Mott transition, where only the plane-perpendicular a1g orbital of the Fe(3d) manifold remains itinerant. Our results highlight the multi-orbital character in Fe3-xGeTe2 that supports a rare coexistence of local and itinerant physics within this material. △ Less

Submitted 11 November, 2022; v1 submitted 28 January, 2022; originally announced January 2022.

Comments: 16 pages, 3 main figures

Journal ref: Phys. Rev. B 106, L180409 (2022)

Tuning the Room Temperature Ferromagnetism in Fe5GeTe2 by Arsenic Substitution

Authors: Andrew F. May, Jiaqiang Yan, Raphael Hermann, Mao-Hua Du, Michael A. McGuire

Abstract: In order to tune the magnetic properties of the cleavable high-Curie temperature ferromagnet Fe$_{5-x}$GeTe$_2$, the effect of increasing the electron count through arsenic substitution has been investigated. Small additions of arsenic (2.5 and 5%) seemingly enhance ferromagnetic order in polycrystalline samples by quenching fluctuations on one of the three magnetic sublattices, whereas larger As… ▽ More In order to tune the magnetic properties of the cleavable high-Curie temperature ferromagnet Fe$_{5-x}$GeTe$_2$, the effect of increasing the electron count through arsenic substitution has been investigated. Small additions of arsenic (2.5 and 5%) seemingly enhance ferromagnetic order in polycrystalline samples by quenching fluctuations on one of the three magnetic sublattices, whereas larger As concentrations decrease the ferromagnetic Curie temperature ($T_{\rm C}$) and saturation magnetization. This work also describes the growth and characterization of Fe$_{4.8}$AsTe$_2$ single crystals that are structurally analogous to Fe$_{5-x}$GeTe$_2$ but with some phase stability complications. Magnetization measurements reveal dominant antiferromagnetic behavior in Fe$_{4.8}$AsTe$_2$ with a Néel temperature of $T_{\rm N}$ $\approx$42K. A field-induced spin-flop below $T_{\rm N}$ results in a switch from negative to positive magnetoresistance, with significant hysteresis causing butterfly-shaped resistance loops. In addition to reporting the properties of Fe$_{4.8}$AsTe$_2$, this work shows the importance of manipulating the individual magnetic sublattices in Fe$_{5-x}$GeTe$_2$ and motivates further efforts to control the magnetic properties in related materials by fine tuning of the Fermi energy or crystal chemistry. △ Less

Submitted 11 November, 2021; originally announced November 2021.

Comments: Accepted for publication in 2D Materials, with accepted version online

Vapor transport growth of MnBi2Te4 and related compounds

Authors: J. -Q. Yan, Z. L. Huang, W. D. Wu, A. F. May

Abstract: Motivated by fine tuning of the magnetic and topological properties of MnBi$_2$Te$_4$ via defect engineering, in this work, we report the crystal growth of MnBi$_2$Te$_4$ and related compounds using vapor transport method and characterization of vapor transported crystals by measuring elemental analysis, magnetic and transport properties, and scanning tunneling microscopy. For the growth of MnBi… ▽ More Motivated by fine tuning of the magnetic and topological properties of MnBi$_2$Te$_4$ via defect engineering, in this work, we report the crystal growth of MnBi$_2$Te$_4$ and related compounds using vapor transport method and characterization of vapor transported crystals by measuring elemental analysis, magnetic and transport properties, and scanning tunneling microscopy. For the growth of MnBi$_2$Te$_4$ single crystals, I$_2$, MnI$_2$ , MnCl$_2$, TeCl$_4$, or MoCl$_5$ are all effective transport agents; chemical transportation occurs faster in the presence of iodides than chlorides. MnBi$_2$Te$_4$ crystals can be obtained in the temperature range 500$^\circ$C-590$^\circ$C using I$_2$ as the transport agent. We further successfully grow MnSb$_2$Te$_4$, MnBi$_{2-x}$Sb$_x$Te$_4$, and Sb-doped MnBi$_4$Te$_7$ crystals. A small temperature gradient $<$20$^\circ$C between the hot and cold ends of the growth cmpoule is critical for the successful crystal growth of MnBi$_2$Te$_4$ and related compounds. Compared to flux grown crystals, vapor transported crystals tend to be Mn stoichiometric, and Sb-bearing compositions have more Mn/Sb site mixing. The vapor transport growth provides a new materials synthesis approach to fine tuning the magnetic and topological properties of these intrinsic magnetic topological insulators. △ Less

Submitted 12 October, 2021; originally announced October 2021.

Comments: all comments/discussions are welcome

Journal ref: Journal of Alloys and Compounds 906, 164327 (2022)

Revealing room temperature ferromagnetism in exfoliated Fe$_5$GeTe$_2$ flakes with quantum magnetic imaging

Authors: Hang Chen, Shahidul Asif, Matthew Whalen, Jeyson Tamara-Isaza, Brennan Luetke, Yang Wang, Xinhao Wang, Millicent Ayako, Saurabh Lamsal, Andrew F. May, Michael A. McGuire, Chitraleema Chakraborty, John Q. Xiao, Mark J. H. Ku

Abstract: Van der Waals material Fe$_5$GeTe$_2$, with its long-range ferromagnetic ordering near room temperature, has significant potential to become an enabling platform for implementing novel spintronic and quantum devices. To pave the way for applications, it is crucial to determine the magnetic properties when the thickness of Fe5GeTe2 reaches the few-layers regime. However, this is highly challenging… ▽ More Van der Waals material Fe$_5$GeTe$_2$, with its long-range ferromagnetic ordering near room temperature, has significant potential to become an enabling platform for implementing novel spintronic and quantum devices. To pave the way for applications, it is crucial to determine the magnetic properties when the thickness of Fe5GeTe2 reaches the few-layers regime. However, this is highly challenging due to the need for a characterization technique that is local, highly sensitive, artifact-free, and operational with minimal fabrication. Prior studies have indicated that Curie temperature TC can reach up to close to room temperature for exfoliated Fe$_5$GeTe$_2$ flakes, as measured via electrical transport; there is a need to validate these results with a measurement that reveals magnetism more directly. In this work, we investigate the magnetic properties of exfoliated thin flakes of van der Waals magnet Fe$_5$GeTe$_2$ via a quantum magnetic imaging technique based on nitrogen vacancy diamond. Through imaging the stray fields, we confirm room-temperature magnetic order in Fe$_5$GeTe$_2$ thin flakes with thickness down to 7 units cell. The stray field patterns and their response to magnetizing fields with different polarities point to a perpendicular easy-axis anisotropy. Furthermore, we perform imaging at different temperatures and determine the Curie temperature of the flakes at Tc~300 K. These results provide the basis for realizing a room-temperature monolayer ferromagnet with Fe$_5$GeTe$_2$. This work also demonstrates that the imaging technique enables a rapid screening of multiple flakes simultaneously, thereby paving the way towards high throughput characterization of potential 2D magnets near room temperature. △ Less

Submitted 20 March, 2022; v1 submitted 11 October, 2021; originally announced October 2021.

Journal ref: 2D Mater. (2022) 9 025017

Photo-induced plasmon-phonon coupling in PbTe

Authors: M. P. Jiang, M. Trigo, S. Fahy, A. Hauber, É. D. Murray, I Savić, C. Bray, J. N. Clark, T. Henighan, M. Kozina, M. Chollet, J. M. Glownia, M. C. Hoffmann, D. Zhu, O. Delaire, A. F. May, B. C. Sales, A. M. Lindenberg, P. Zalden, T. Sato, R. Merlin, D. A. Reis

Abstract: We report the observation of photo-induced plasmon-phonon coupled modes in the group IV-VI semiconductor PbTe using Fourier-transform inelastic X-ray scattering at the Linac Coherent Light Source (LCLS). We measure the near-zone-center dispersion of the heavily screened longitudinal optical (LO) phonon branch as extracted from differential changes in x-ray diffuse scattering intensity following ab… ▽ More We report the observation of photo-induced plasmon-phonon coupled modes in the group IV-VI semiconductor PbTe using Fourier-transform inelastic X-ray scattering at the Linac Coherent Light Source (LCLS). We measure the near-zone-center dispersion of the heavily screened longitudinal optical (LO) phonon branch as extracted from differential changes in x-ray diffuse scattering intensity following above band gap photoexcitation. △ Less

Submitted 3 September, 2021; originally announced September 2021.

Comments: 5 pages, 2 figures

Synthesis and Anisotropic Magnetism in Quantum Spin Liquid Candidates $A$YbSe$_2$ ($A$ = K and Rb)

Authors: Jie Xing, Liurukara D. Sanjeewa, Andrew F. May, Athena S. Sefat

Abstract: Quantum spin liquid (QSL) state in rare-earth triangular lattice has attracted much attention recently due to its potential application in quantum computing and communication. Here we report the single-crystal growth synthesis, crystal structure characterizations and magnetic properties of $A$YbSe$_{2}$ ($A$= K, Rb) compounds. The X-ray diffraction analysis shows that $A$YbSe$_{2}$ ($A$ = K and Rb… ▽ More Quantum spin liquid (QSL) state in rare-earth triangular lattice has attracted much attention recently due to its potential application in quantum computing and communication. Here we report the single-crystal growth synthesis, crystal structure characterizations and magnetic properties of $A$YbSe$_{2}$ ($A$= K, Rb) compounds. The X-ray diffraction analysis shows that $A$YbSe$_{2}$ ($A$ = K and Rb) crystallizes in a trigonal space group, $R$-3$m$ (No. 166) with Z = 3. $A$YbSe$_{2}$ possesses a two-dimensional (2D) Yb-Se-Yb layered structure formed by edged-shared YbSe$_6$ octahedra. The magnetic properties are highly anisotropic for both title compounds and no long-range order is found down to 0.4 K, revealing the possible QSL ground state in these compounds. The isothermal magnetization exhibits one-third magnetization plateau when the magnetic fields are applied in $ab$-plane. Heat capacity is performed along both $ab$-plane and $c$-axis, and features the characteristic dome for triangular magnetic lattice compounds as a function of magnetic fields. Due to the change of the interlayer and intralayer distance of Yb$^{3+}$, the dome shifts to low fields from KYbSe$_2$ to RbYbSe$_2$. All these results indicate the $A$YbSe$_2$ family presents unique frustrated magnetism close to the possible QSL and noncolinear spin states. △ Less

Submitted 9 September, 2021; v1 submitted 1 September, 2021; originally announced September 2021.

Comments: 9 pages, 7 figures

Journal ref: APL Mater. 9, 111104 (2021)

Tuning the flat bands of the kagome metal CoSn with Fe, In, or Ni doping

Authors: B. C. Sales, W. R. Meier, A. F. May, J. Xing, J. -Q Yan, S. Gao, Y. H. Liu, M. B. Stone, A. D. Christianson, Q. Zhang, M. A. McGuire

Abstract: CoSn is a Pauli paramagnet with relatively flat d-bands centered about 100 meV below the Fermi energy Ef. Single crystals of CoSn lightly doped with Fe, In, or Ni are investigated using x-ray and neutron scattering, magnetic susceptibility and magnetization, ac susceptibility, specific heat and resistivity measurements. Within the rigid band approximation, hole doping with a few percent of Fe or I… ▽ More CoSn is a Pauli paramagnet with relatively flat d-bands centered about 100 meV below the Fermi energy Ef. Single crystals of CoSn lightly doped with Fe, In, or Ni are investigated using x-ray and neutron scattering, magnetic susceptibility and magnetization, ac susceptibility, specific heat and resistivity measurements. Within the rigid band approximation, hole doping with a few percent of Fe or In should move the flat bands closer to Ef, whereas electron doping with Ni should move the flat bands further away from Ef. We provide evidence that this indeed occurs. Fe and In doping drive CoSn toward magnetism, while Ni doping suppresses CoSn's already weak magnetic response. The resulting ground state is different for Fe versus In doping. For Fe-doped crystals, Co1-xFexSn, with 0.02 < x < 0.27, the magnetic and specific heat data are consistent with the formation of a spin glass, with a glass transition temperature, Tg, ranging from 1 K for x=0.02 to 10 K for x= 0.27. Powder and single crystal neutron diffraction found no evidence of long-range magnetic order below Tg with x = 0.17. For In-doped crystals, CoSn1-yIny, both the magnetic susceptibility and the Sommerfeld coefficient, gamma, increase substantially relative to pure CoSn, but with no clear indication of a magnetic transition for 0.05 < y < 0.2. CoSn crystals doped with Ni (Co0.93Ni0.07Sn) have a significantly smaller magnetic susceptibility and gamma than pure CoSn, consistent with the flat bands further from Ef. △ Less

Submitted 17 February, 2021; originally announced February 2021.

Comments: 20 pages, 10 figures

Journal ref: Phys. Rev. Materials 5, 044202 (2021)

Hierarchical excitations from correlated spin tetrahedra on the breathing pyrochlore lattice

Authors: Shang Gao, Andrew F. May, Mao-Hua Du, Joseph A. M. Paddison, Hasitha Suriya Arachchige, Ganesh Pokharel, Clarina dela Cruz, Qiang Zhang, Georg Ehlers, David S. Parker, David G. Mandrus, Matthew B. Stone, Andrew D. Christianson

Abstract: The hierarchy of the coupling strengths in a physical system often engenders an effective model at low energies where the decoupled high-energy modes are integrated out. Here, using neutron scattering, we show that the spin excitations in the breathing pyrochlore lattice compound CuInCr$_4$S$_8$ are hierarchical and can be approximated by an effective model of correlated tetrahedra at low energies… ▽ More The hierarchy of the coupling strengths in a physical system often engenders an effective model at low energies where the decoupled high-energy modes are integrated out. Here, using neutron scattering, we show that the spin excitations in the breathing pyrochlore lattice compound CuInCr$_4$S$_8$ are hierarchical and can be approximated by an effective model of correlated tetrahedra at low energies. At higher energies, intra-tetrahedron excitations together with strong magnon-phonon couplings are observed, which suggests the possible role of the lattice degree of freedom in stabilizing the spin tetrahedra. Our work illustrates the spin dynamics in CuInCr$_4$S$_8$ and demonstrates a general effective-cluster approach to understand the dynamics on the breathing-type lattices. △ Less

Submitted 28 January, 2021; originally announced January 2021.

Comments: 11 pages, 9 figures

Journal ref: Phys. Rev. B 103, 214418 (2021)

Complex magnetic phases in polar tetragonal intermetallic NdCoGe$_3$

Authors: Binod K. Rai, Ganesh Pokharel, Hasitha Suriya Arachchige, Seung-Hwan Do, Qiang Zhang, Masaaki Matsuda, Matthias Frontzek, Gabriele Sala, V. Ovidiu Garlea, Andrew D. Christianson, Andrew F. May

Abstract: Polar materials can host a variety of topologically significant magnetic phases, which often emerge from a modulated magnetic ground state. Relatively few noncentrosymmetric tetragonal materials have been shown to host topological spin textures and new candidate materials are necessary to expand the current theoretical models. This manuscript reports on the anisotropic magnetism in the polar, tetr… ▽ More Polar materials can host a variety of topologically significant magnetic phases, which often emerge from a modulated magnetic ground state. Relatively few noncentrosymmetric tetragonal materials have been shown to host topological spin textures and new candidate materials are necessary to expand the current theoretical models. This manuscript reports on the anisotropic magnetism in the polar, tetragonal material NdCoGe$_3$ via thermodynamic and neutron diffraction measurements. The previously reported $H$-$T$ phase diagram is updated to include several additional phases, which exist for both $H$ = 0 and with an applied field H$\perp$ c. Neutron diffraction data reveal that the magnetic structures below $T_{N1}$ = 3.70 K and $T_{N2}$ = 3.50 K are incommensurate, with a ground state magnetic order that is incommensurate in all directions with the propagation vector $\vec{k}$ = (0.494, 0.0044, 0.385) at 1.8 K. A unique magnetic structure solution is not achievable, but the possible single and multi-$\vec{k}$ spin models are discussed. These results demonstrate that NdCoGe3 hosts complicated magnetic order derived from modulated magnetic moments. △ Less

Submitted 18 December, 2020; originally announced December 2020.

Comments: 11 pages, 10 figures

Journal ref: Phys. Rev. B 103, 014426 (2021)

Weakly coupled alternating $S=1/2$ chains in the distorted honeycomb lattice compound Na$_2$Cu$_2$TeO$_6$

Authors: Shang Gao, Ling-Fang Lin, Andrew F. May, Binod K. Rai, Qiang Zhang, Elbio Dagotto, Andrew D. Christianson, Matthew B. Stone

Abstract: Spin-1/2 chains with alternating antiferromagnetic (AF) and ferromagnetic (FM) couplings exhibit quantum entanglement like the integer-spin Haldane chains and might be similarly utilized for quantum computations. Such alternating AF-FM chains have been proposed to be realized in the distorted honeycomb-lattice compound Na$_2$Cu$_2$TeO$_6$, but to confirm this picture a comprehensive understanding… ▽ More Spin-1/2 chains with alternating antiferromagnetic (AF) and ferromagnetic (FM) couplings exhibit quantum entanglement like the integer-spin Haldane chains and might be similarly utilized for quantum computations. Such alternating AF-FM chains have been proposed to be realized in the distorted honeycomb-lattice compound Na$_2$Cu$_2$TeO$_6$, but to confirm this picture a comprehensive understanding of the exchange interactions including terms outside of the idealized model is required. Here we employ neutron scattering to study the spin dynamics in Na$_2$Cu$_2$TeO$_6$ and accurately determine the coupling strengths through the random phase approximation and density functional theory (DFT) approaches. We find the AF and FM intrachain couplings are the dominant terms in the spin Hamiltonian, while the interchain couplings are AF but perturbative. This hierarchy in the coupling strengths and the alternating signs of the intrachain couplings can be understood through their different exchange paths. Our results establish Na$_2$Cu$_2$TeO$_6$ as a weakly-coupled alternating AF-FM chain compound and reveal the robustness of the gapped ground state in alternating chains under weak interchain couplings. △ Less

Submitted 7 December, 2020; v1 submitted 13 October, 2020; originally announced October 2020.

Comments: 9 pages, 7 figures

Journal ref: Phys. Rev. B 102, 220402(R) (2020)