arXiv subjects

Andrew F. May

Publications and source records attributed to Andrew F. May.

At least 55 records · Page 3Linked to original sources

arXiv2021

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

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.

cond-mat.str-el↗

arXiv2021

Hierarchical excitations from correlated spin tetrahedra on the breathing pyrochlore lattice

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.

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arXiv2020

Complex magnetic phases in polar tetragonal intermetallic NdCoGe$_3$

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.

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arXiv2020

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

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.

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arXiv2020

Interlayer magnetism in Fe3-xGeTe2

Fe$_{3-x}$GeTe$_2$ is a layered van der Waals magnetic material with a relatively high ordering temperature and large anisotropy. While most studies have concluded the interlayer ordering to be ferromagnetic, there have also been reports of interlayer antiferromagnetism in Fe$_{3-x}$GeTe$_2$. Here, we investigate the interlayer magnetic ordering by neutron diffraction experiments, scanning tunneling microscopy (STM) and spin-polarized STM measurements, density functional theory plus U calculations and STM simulations. We conclude that the layers of Fe$_{3-x}$GeTe$_2$ are coupled ferromagnetically and that in order to capture the magnetic and electronic properties of Fe$_{3-x}$GeTe$_2$ within density functional theory, Hubbard U corrections need to be taken into account.

cond-mat.mtrl-sci↗

arXiv2020

Tuning Magnetic Order in the van der Waals Metal Fe5GeTe2 by Cobalt Substitution

Fe5-xGeTe2 is a van der Waals material with one of the highest reported bulk Curie temperatures, $T_C$ ~ 310K. In this study, theoretical calculations and experiments are utilized to demonstrate that the magnetic ground state is highly sensitive to local atomic arrangements and the interlayer stacking. Cobalt substitution is found to be an effective way to manipulate the magnetic properties while also increasing the ordering temperature. In particular, cobalt substitution up to 30% enhances $T_C$ and changes the magnetic anisotropy, while approximately 50% cobalt substitution yields an antiferromagnetic state. Single crystal x-ray diffraction evidences a structural change upon increasing the cobalt concentration, with a rhombohedral cell observed in the parent material and a primitive cell observed for ~46% cobalt content relative to iron. First principles calculations demonstrate that it is a combination of high cobalt content and the concomitant change to primitive layer stacking that produces antiferromagnetic order. These results illustrate the sensitivity of magnetism in Fe5-xGeTe2 to composition and structure, and emphasize the important role of structural order/disorder and layer stacking in cleavable magnetic materials.

cond-mat.mtrl-sci↗

arXiv2020

Fantastic flat bands and where to find them: The CoSn-type compounds

Quantum interference on the kagome lattice generates electronic bands with narrow bandwidth, called flat bands. Crystal structures incorporating this lattice can host strong electron correlations with non-standard ingredients, but only if these bands lie at the Fermi level. In the six compounds with the CoSn structure type (FeGe, FeSn, CoSn, NiIn, RhPb, and PtTl) the transition metals form a kagome lattice. The two iron variants are robust antiferromagnets so we focus on the latter four and investigate their thermodynamic and transport properties. We consider these results and calculated band structures to locate and characterize the flat bands in these materials. We propose that CoSn and RhPb deserve the community's attention for exploring flat band physics.

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arXiv2020

Physical properties and thermal stability of Fe5GeTe2 single crystals

The magnetic and transport properties of Fe-deficient Fe5GeTe2 single crystals (Fe5-xGeTe2 with x~0.3) were studied and the impact of thermal processing was explored. Quenching crystals from the growth temperature has been previously shown to produce a metastable state that undergoes a strongly hysteretic first-order transition upon cooling below ~100K. The first-order transition impacts the magnetic properties, yielding an enhancement in the Curie temperature T_C from 270 to 310K. In the present work, T_HT ~550K has been identified as the temperature above which metastable crystals are obtained via quenching. Diffraction experiments reveal a structural change at this temperature, and significant stacking disorder occurs when samples are slowly cooled through this temperature range. The transport properties are demonstrated to be similar regardless of the crystal's thermal history. The scattering of charge carriers appears to be dominated by moments fluctuating on the Fe(1) sublattice, which remain dynamic down to 100-120K. Maxima in the magnetoresistance and anomalous Hall resistance are observed near 120K. The Hall and Seebeck coefficients are also impacted by magnetic ordering on the Fe(1) sublattice. The data suggest that both electrons and holes contribute to conduction above 120K, but that electrons dominate at lower temperature when all of the Fe sublattices are magnetically ordered. This study demonstrates a strong coupling of the magnetism and transport properties in Fe5-xGeTe2 and complements the previous results that demonstrated strong magnetoelastic coupling as the Fe(1) moments order. The published version of this manuscript is DOI:10.1103/PhysRevMaterials.3.104401 (2019)

cond-mat.mtrl-sci↗

arXiv2020

Cluster Frustration in the Breathing Pyrochlore Magnet LiGaCr4S8

We present a comprehensive neutron scattering study of the breathing pyrochlore magnet LiGaCr4S8. We observe an unconventional magnetic excitation spectrum with a separation of high and low-energy spin dynamics in the correlated paramagnetic regime above a spin-freezing transition at 12(2) K. By fitting to magnetic diffuse-scattering data, we parameterize the spin Hamiltonian. We find that interactions are ferromagnetic within the large and small tetrahedra of the breathing pyrochlore lattice, but antiferromagnetic further-neighbor interactions are also essential to explain our data, in qualitative agreement with density-functional theory predictions [Ghoshet al.,npj Quantum Mater.4, 63 (2019)]. We explain the origin of geometrical frustration in LiGaCr4S8 interms of net antiferromagnetic coupling between emergent tetrahedral spin clusters that occupy a face-centered lattice. Our results provide insight into the emergence of frustration in the presence of strong further-neighbor couplings, and a blueprint for the determination of magnetic interactions in classical spin liquids.

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arXiv2019

Synthesis, magnetization and heat capacity of triangular lattice materials NaErSe$_2$ and KErSe$_2$

In this paper we report the synthesis, magnetization and heat capacity of the frustrated magnets \emph{A}ErSe$_2$(\emph{A}=Na,K) which contain perfect triangular lattices of Er$^{3+}$. The magnetization data suggests no long-range magnetic order exists in \emph{A}ErSe$_2$(\emph{A}=Na,K), which is consistent with the heat capacity measurements. Large anisotropy is observed between the magnetization within the \emph{ab} plane and along the \emph{c} axis of both compounds. When the magnetic field is applied along \emph{ab} plane, anomalies are observed at 1.8 $μ_B$ in NaErSe$_2$ at 0.2 T and 2.1 $μ_B$ in KErSe$_2$ at 0.18 T. Unlike NaErSe$_2$, a plateau-like field-induced metamagnetic transition is observed for H$\|$\emph{c} below 1 K in KErSe$_2$. Two broad peaks are observed in the heat capacity below 10 K indicating possible crystal electric field(CEF) effects and magnetic entropy released under different magnetic fields. All results indicate that \emph{A}ErSe$_2$ are strongly anisotropic, frustrated magnets with field-induced transition at low temperature. The lack of signatures for long-range magnetic order implies that these materials are candidates for hosting a quantum spin liquid ground state.

cond-mat.mtrl-sci↗

arXiv2019

Influence of cobalt substitution on the magnetism of NiBr$_2$

Co substituted Ni$_{1-x}$Co$_x$Br$_2$ (0 $\leq~x~\leq$ 1) single crystals were synthesized using vapor transport. The physical properties of the crystals were characterized by x-ray powder diffraction, magnetization, and specific heat measurements. Room temperature x-ray powder diffraction data indicate a change from the CdCl$_2$ structure type to the CdI$_2$ structure type occurs within 0.56 $<~x~<$ 0.76. NiBr$_2$ has a commensurate antiferromagnetic phase below $T_{\rm N} \approx$ 46 K and an incommensurate magnetic ground state below $T_{\rm IC} \approx$ 20 K. Both magnetic transitions are affected by cobalt substitution, and the incommensurate phase transition is present up to at least $x$ = 0.56. The evolution of magnetism has been studied as a function of cobalt content and is summarized in the temperature-composition phase diagram.

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arXiv2018

Single Crystal High Entropy Perovskite Oxide Epitaxial Films

The first examples of single crystal epitaxial thin films of a high entropy perovskite oxide are synthesized. Pulsed laser deposition is used to grow the configurationally disordered ABO3 perovskite, Ba(Zr0.2Sn0.2Ti0.2Hf0.2Nb0.2)O3, epitaxially on SrTiO3 and MgO substrates. X-ray diffraction and scanning transmission electron microscopy demonstrate that the films are single phase with excellent crystallinity and atomically abrupt interfaces to the underlying substrates. Atomically-resolved electron energy loss spectroscopy mapping shows a uniform and random distribution of all B-site cations. The ability to stabilize perovskites with this level of configurational disorder offers new possibilities for designing materials from a much broader combinatorial cation pallet while providing a fresh avenue for fundamental studies in strongly correlated quantum materials where local disorder can play a critical role in determining macroscopic properties.

cond-mat.mtrl-sci↗

arXiv2018

Model-free reconstruction of magnetic correlations in frustrated magnets

Frustrated magnetic systems exhibit extraordinary physical properties but quantification of their magnetic correlations poses a serious challenge to experiment and theory. Current insight into frustrated magnetic correlations relies on modelling techniques such as reverse Monte Carlo methods, which require knowledge about the exact ordered atomic structure. Here we present a method for direct reconstruction of magnetic correlations in frustrated magnets by three-dimensional difference pair distribution function analysis of neutron total scattering data. The methodology is applied to the disordered frustrated magnet bixbyite, (Mn1-xFex)2O3, which reveals nearest-neighbor antiferromagnetic correlations for the metal sites up to a range of approximately 15 Å. Importantly, this technique allows for magnetic correlations to be determined directly from the experimental data without any assumption about the atomic structure.

cond-mat.mtrl-sci↗

arXiv2017

High-temperature magnetostructural transition in van der Waals-layered a-MoCl3

The crystallographic and magnetic properties of the cleavable 4d3 transition metal compound a-MoCl3 are reported, with a focus on the behavior above room temperature. Crystals were grown by chemical vapor transport and characterized using temperature dependent x-ray diffraction, Raman spectroscopy, and magnetization measurements. A structural phase transition occurs near 585 K, at which the Mo-Mo dimers present at room temperature are broken. A nearly regular honeycomb net of Mo is observed above the transition, and an optical phonon associated with the dimerization instability is identified in the Raman data and in first-principles calculations. The crystals are diamagnetic at room temperature in the dimerized state, and the magnetic susceptibility increases sharply at the structural transition. Moderately strong paramagnetism in the high-temperature structure indicates the presence of local moments on Mo. This is consistent with results of spin-polarized density functional theory calculations using the low- and high-temperature structures. Above the magnetostructural phase transition the magnetic susceptibility continues to increase gradually up to the maximum measurement temperature of 780 K, with a temperature dependence that suggests two-dimensional antiferromagnetic correlations.

cond-mat.mtrl-sci↗

arXiv2017

Magnetic order and interactions in ferrimagnetic Mn3Si2Te6

The magnetism in Mn$_3$Si$_2$Te$_6$ has been investigated using thermodynamic measurements, first principles calculations, neutron diffraction and diffuse neutron scattering on single crystals. These data confirm that Mn$_3$Si$_2$Te$_6$ is a ferrimagnet below a Curie temperature of $T_C$ approximately 78K. The magnetism is anisotropic, with magnetization and neutron diffraction demonstrating that the moments lie within the basal plane of the trigonal structure. The saturation magnetization of approximately 1.6$μ_B$/Mn at 5K originates from the different multiplicities of the two antiferromagnetically-aligned Mn sites. First principles calculations reveal antiferromagnetic exchange for the three nearest Mn-Mn pairs, which leads to a competition between the ferrimagnetic ground state and three other magnetic configurations. The ferrimagnetic state results from the energy associated with the third-nearest neighbor interaction, and thus long-range interactions are essential for the observed behavior. Diffuse magnetic scattering is observed around the 002 Bragg reflection at 120K, which indicates the presence of strong spin correlations well above $T_C$. These are promoted by the competing ground states that result in a relative suppression of $T_C$, and may be associated with a small ferromagnetic component that produces anisotropic magnetism below $\approx$330K.

cond-mat.str-el↗

arXiv2017

Quantum Critical Behavior in the Asymptotic Limit of High Disorder: Entropy Stabilized NiCoCr0.8 Alloys

The behavior of matter near a quantum critical point (QCP) is one of the most exciting and challenging areas of physics research. Emergent phenomena such as high-temperature superconductivity are linked to the proximity to a QCP. Although significant progress has been made in understanding quantum critical behavior in some low dimensional magnetic insulators, the situation in metallic systems is much less clear. Here we demonstrate that NiCoCrx single crystal alloys are remarkable model systems for investigating QCP physics in a metallic environment. For NiCoCrx alloys with x = 0.8, the critical exponents associated with a ferromagnetic quantum critical point (FQCP) are experimentally determined from low temperature magnetization and heat capacity measurements. For the first time, all of the five critical exponents ( gamma-subT =1/2 , beta-subT = 1, delta = 3/2, nuz-subm = 2, alpha-bar-subT = 0) are in remarkable agreement with predictions of Belitz-Kirkpatrick-Vojta (BKV) theory in the asymptotic limit of high disorder. Using these critical exponents, excellent scaling of the magnetization data is demonstrated with no adjustable parameters. We also find a divergence of the magnetic Gruneisen parameter, consistent with a FQCP. This work therefore demonstrates that entropy stabilized concentrated solid solutions represent a unique platform to study quantum critical behavior in a highly tunable class of materials.

cond-mat.str-el↗

arXiv2016

Competing magnetic ground states and their coupling to the crystal lattice in CuFe2Ge2

Identifying and characterizing systems with coupled and competing interactions is central to the development of physical models that can accurately describe and predict emergent behavior in condensed matter systems. This work demonstrates that the metallic compound CuFe$_2$Ge$_2$ has competing magnetic ground states, which are shown to be strongly coupled to the lattice and easily manipulated using temperature and applied magnetic fields. Temperature-dependent magnetization $M$ measurements reveal a ferromagnetic-like onset at 228(1)\,K and a broad maximum in $M$ near 180\,K. Powder neutron diffraction confirms antiferromagnetic ordering below $T_{\textrm{N}}\approx$175\,K, and an incommensurate spin density wave is observed below $\approx$125\,K. Coupled with the small refined moments (0.5-1\,$μ_B$/Fe), this provides a picture of itinerant magnetism in CuFe$_2$Ge$_2$. The neutron diffraction data also reveal a coexistence of two magnetic phases that further highlights the near-degeneracy of various magnetic states. These results demonstrate that the ground state in CuFe$_2$Ge$_2$ can be easily manipulated by external forces, making it of particular interest for doping, pressure, and further theoretical studies.

cond-mat.str-el↗

arXiv2016

Phonon anharmonicity and negative thermal expansion in SnSe

The anharmonic phonon properties of SnSe in the Pnma phase were investigated with a combination of experiments and first-principles simulations. Using inelastic neutron scattering (INS) and nuclear resonant inelastic X-ray scattering (NRIXS), we have measured the phonon dispersions and density of states (DOS) and their temperature dependence, which revealed a strong, inhomogeneous shift and broadening of the spectrum on warming. First-principles simulations were performed to rationalize these measurements, and to explain the previously reported anisotropic thermal expansion, in particular the negative thermal expansion within the Sn-Se bilayers. Including the anisotropic strain dependence of the phonon free energy, in addition to the electronic ground state energy, is essential to reproduce the negative thermal expansion. From the phonon DOS obtained with INS and additional calorimetry measurements, we quantify the harmonic, dilational, and anharmonic components of the phonon entropy, heat capacity, and free energy. The origin of the anharmonic phonon thermodynamics is linked to the electronic structure.

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