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Topological materials hosting kagome lattices have drawn considerable attention due to the interplay between topology, magnetism, and electronic correlations. The (Fe$_{1-x}$Co$_x$)Sn system not only hosts a kagome lattice but has a tunable symmetry breaking magnetic moment with temperature and doping. In this study, angle resolved photoemission spectroscopy and first principles calculations are used to investigate the interplay between the topological electronic structure and varying magnetic moment from the planar to axial antiferromagnetic phases. A theoretically predicted gap at the Dirac point is revealed in the low temperature axial phase but no gap opening is observed across a temperature dependent magnetic phase transition. However, topological surface bands are observed to shift in energy as the surface magnetic moment is reduced or becomes disordered over time during experimental measurements. The shifting surface bands may preclude the determination of a temperature dependent bulk gap but highlights the intricate connections between magnetism and topology with a surface/bulk dichotomy that can affect material properties and their interrogation., Comment: 11 pages, 4 figures

The kagome lattice is a fertile platform to explore topological excitations with both Fermi-Dirac and Bose-Einstein statistics. While relativistic Dirac Fermions and flat-bands have been discovered in the electronic structure of kagome metals, the spin excitations have received less attention. Here we report inelastic neutron scattering studies of the prototypical kagome magnetic metal FeSn. The spectra display well-defined spin waves extending up to 120 meV. Above this energy, the spin waves become progressively broadened, reflecting interactions with the Stoner continuum. Using linear spin wave theory, we determine an effective spin Hamiltonian that reproduces the measured dispersion. This analysis indicates that the Dirac magnon at the K-point remarkably occurs on the brink of a region where well-defined spin waves become unobservable. Our results emphasize the influential role of itinerant carriers on the topological spin excitations of metallic kagome magnets., 6 pages, 4 figures

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$_{4}$., 20 pages, 15 figures

Kagome lattices host flat bands due to their frustrated lattice geometry, which leads to destructive quantum interference of electron wave functions. Here, we report imaging of the kagome flat band localization in real-space using scanning tunneling microscopy. We identify both the Fe3Sn kagome lattice layer and the Sn2 honeycomb layer with atomic resolution in kagome antiferromagnet FeSn. On the Fe3Sn lattice, at the flat band energy determined by the angle resolved photoemission spectroscopy, tunneling spectroscopy detects an unusual state localized uniquely at the Fe kagome lattice network. We further show that the vectorial in-plane magnetic field manipulates the spatial anisotropy of the localization state within each kagome unit cell. Our results are consistent with the real-space flat band localization in the magnetic kagome lattice. We further discuss the magnetic tuning of flat band localization under the spin-orbit coupled magnetic kagome lattice model., Comment: To appear in Communications Materials

Fabricating a bonded magnet with a near‐net shape in suitable thermoplastic polymer binders is of paramount importance in the development of cost‐effective energy technologies. In this work, anisotropic Sm2Fe17N3 (Sm–Fe–N) bonded magnets are additively printed using SmFeN anisotropic magnetic particles in a polymeric binder polyamide‐12 (PA12). The anisotropic SmFeN bonded magnets are fabricated by Big Area Additive Manufacturing followed by post‐printing alignment in a magnetic field. Optimal post‐alignment results in an enhanced remanence of ∼0.68 T in PA12 reflected in a parallel‐oriented (aligned) measured direction. The maximum energy product achieved for the additively printed anisotropic bonded magnet of Sm–Fe–N in PA12 polymer is 78.8 KJ m−3. Our results show advanced processing flexibility with 3D printing of the development of SmFeN nylon bonded magnets designed for applications with no critical rare earth magnets.

Single crystals of the underscreened Kondo ferromagnet Yb14MnSb11 were investigated using polarised neutron diffraction and magnetisation measurements. The magnitude and direction of the ma...

Anionic electron within an electride was visualized with atomic resolution using differential phase-contrast imaging., Electrides are an unusual family of materials that feature loosely bonded electrons that occupy special interstitial sites and serve as anions. They are attracting increasing attention because of their wide range of exotic physical and chemical properties. Despite the critical role of the anionic electrons in inducing these properties, their presence has not been directly observed experimentally. Here, we visualize the columnar anionic electron density within the prototype electride Y5Si3 with sub-angstrom spatial resolution using differential phase-contrast imaging in a scanning transmission electron microscope. The data further reveal an unexpected charge variation at different anionic sites. Density functional theory simulations show that the presence of trace H impurities is the cause of this inhomogeneity. The visualization and quantification of charge inhomogeneities in crystals will serve as valuable input in future theoretical predictions and experimental analysis of exotic properties in electrides and materials beyond.

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., 20 pages, 10 figures

Charge density waves (CDW) are modulations of the electron density and the atomic lattice that develop in some crystalline materials at low temperature. We report an unusual example of a CDW in BaFe$_2$Al$_9$ below 100 K. In contrast to the canonical CDW phase transition, temperature dependent physical properties of single crystals reveal a first-order phase transition. This is accompanied by a discontinuous change in the size of the crystal lattice. In fact, this large strain has catastrophic consequences for the crystals causing them to physically shatter. Single crystal x-ray diffraction reveals super-lattice peaks in the low-temperature phase signaling the development of a CDW lattice modulation. No similar low-temperature transitions are observed in BaCo$_2$Al$_9$. Electronic structure calculations provide one hint to the different behavior of these two compounds; the d-orbital states in the Fe compound are not completely filled. Iron compounds are renowned for their magnetism and partly filled d-states play a key role. It is therefore surprising that BaFe$_2$Al$_9$ develops a structural modulation instead at low temperature instead of magnetic order., 34 pages, 8 figures Edits to text as well as figures 2 and 5. Added neutron diffraction (Fig. 6)

Summary Thermoelectric modules are a promising approach to energy harvesting and efficient cooling. In addition to the longitudinal Seebeck effect, transverse devices utilizing the anomalous Nernst effect (ANE) have recently attracted interest. For high conversion efficiency, it is required that the material have a large ANE thermoelectric power and low electrical resistance, which lead to the conductivity of the ANE. ANE is usually explained in terms of intrinsic contributions from Berry curvature. Our observations suggest that extrinsic contributions also matter. Studying single-crystal manganese-bismuth (MnBi), we find a high ANE thermopower (∼10 μV/K) under 0.6 T at 80 K, and a transverse thermoelectric conductivity of over 40 A/Km. With insight from theoretical calculations, we attribute this large ANE predominantly to a new advective magnon contribution arising from magnon-electron spin-angular momentum transfer. We propose that introducing a large spin-orbit coupling into ferromagnetic materials may enhance the ANE through the extrinsic contribution of magnons., Graphical abstract, Highlights • MnBi shows a remarkable anomalous Nernst thermopower of 10 μV/K at 80 K • Anomalous Nernst conductivity reaches 40 A/Km, the highest value reported • Magnon-electron drag is likely the source of the large anomalous Nernst effect, Context & scale Thermoelectricity offers the prospect of generating electric power from heat and controlling temperatures in a directed manner. The oldest thermoelectric devices, dating to the 1800s, were based on Seebeck’s observation of electric fields forming in the direction of a temperature gradient. More recent devices have been based on the transverse thermoelectric effect, in which the voltage and thermal gradients are perpendicular. In the anomalous Nernst effect, a magnetic field normal to a thermal gradient produces a voltage drop transverse to both. This Hall-like effect is poorly understood but has great potential for applications in thermoelectric energy harvesting and cooling. We demonstrate a startlingly large transverse thermoelectric response in MnBi crystals, which traditional approaches cannot fully explain. We believe that it is due to interactions between magnons and electrons. This mechanism may operate in other materials, allowing major advances in thermoelectrics., Transverse thermoelectrics utilizing the anomalous Nernst effect (ANE) can be a novel approach to energy sustainability. We investigate the thermoelectric transport properties in ferromagnetic MnBi and observe one of the largest ANEs ever reported. We attribute this giant ANE to the coexistence of ferromagnetism and the heavy Bi atom. Our discovery proposes an alternative recipe to generate large ANE, which introduce a large spin-orbit coupling to ferromagnetic systems.

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 nonstandard 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.

The van der Waals compound, MnBi$_2$Te$_4$, is the first intrinsic magnetic topological insulator, providing a materials platform for exploring exotic quantum phenomena such as the axion insulator state and the quantum anomalous Hall effect. However, intrinsic structural imperfections lead to bulk conductivity, and the roles of magnetic defects are still unknown. With higher concentrations of same types of magnetic defects, the isostructural compound MnSb$_2$Te$_4$ is a better model system for a systematic investigation of the connections among magnetic, topology and lattice defects. In this work, the impact of antisite defects on the magnetism and electronic structure is studied in MnSb$_2$Te$_4$. Mn-Sb site mixing leads to complex magnetic structures and tunes the interlayer magnetic coupling between antiferromagnetic and ferromagnetic. The detailed nonstoichiometry and site-mixing of MnSb$_2$Te$_4$ crystals depend on the growth parameters, which can lead to $\approx$40\% of Mn sites occupied by Sb and $\approx$15\% of Sb sites by Mn in as-grown crystals. Single crystal neutron diffraction and electron microscopy studies show nearly random distribution of the antisite defects. Band structure calculations suggest that the Mn-Sb site-mixing favors a FM interlayer coupling, consistent with experimental observation, but is detrimental to the band inversion required for a nontrivial topology. Our results suggest a long range magnetic order of Mn ions sitting on Bi sites in MnBi$_2$Te$_4$. The effects of site mixing should be considered in all layered heterostructures that consist of alternating magnetic and topological layers, including the entire family of MnTe(Bi$_2$Te$_3$)$_n$, its Sb analogs and their solid solution., The effects of Mn/Sb antisite mixing on the magnetic structure (experiment) and band topology (theory) in the van der Waals magnet MnSb$_2$Te$_4$. PRX in press

This theoretical and experimental work finds the simple CsCl-structure TlBr to exhibit both high and extremely low thermal conductivity in different temperature ranges. First-principles calculations demonstrate that low room-temperature lattice thermal conductivity arises from avoided-crossing-related anharmonicity (only effective at appreciable temperatures) and multiple related lattice near instabilities. Evidence for `localized oscillator' thermal transport, originally hypothesized by Einstein, is also presented.

Correlated quantum materials are expected to provide the foundation for the next generation of information or energy technologies. A key feature of these materials is the proximity of multiple grou...

Triple-layered Sr4Ru3O10 is a unique ferromagnet with the central RuO6 layer behaving differently from two outer layers both crystallographically and magnetically. We report that the partial substitution of Ru by smaller Mn gives rise to modification in crystal structure, electronic and magnetic properties of Sr4(Ru1−xMnx)3O10. Through the single crystal X-ray diffraction refinement, we find that (Ru/Mn)O6 octahedral rotation is no longer detectable at x ≥ 0.23, leading to the tetragonal structure. The magnetization measurements indicate the ferromagnetic transition temperature TC decreases from 105 K for x = 0 to 30 K for x = 0.41, with the reduced magnetic moment as well. Remarkably, Mn doping results in the change of magnetic anisotropy from the easy c axis in x = 0 to the easy ab plane seen in x = 0.34 and 0.41. Such change also removes the ab-plane metamagnetic transition observed in x = 0. Furthermore, the electrical resistivity increases with increasing x showing semiconducting behavior with Δ ~ 10 meV for x = 0.34 and 30 meV for x = 0.41. Under applied magnetic field, the magnetoresistance exhibits negative and linear field dependence in all current and field configurations. These results clearly indicate Sr4(Ru1−xMnx)3O10 is a novel ferromagnetic semiconductor with exotic magnetotransport properties.

Glass-like and crystal-like Crystals with glass-like ultralow thermal conductivity are appealing as barrier coatings and thermoelectric materials. Mukhopadhyay et al. developed a class of thallium selenides with glass-like thermal conductivity. These materials may be promising for applications, but they also require the combination of glass-like and crystal-like thermal transport to explain their thermal properties. This two-channel model can be used to identify potential ultralow-thermal-conductivity compounds. Science , this issue p. 1455

Magnetically isotropic bonded magnets with a high loading fraction of 70 vol.% Nd-Fe-B are fabricated via an extrusion-based additive manufacturing, or 3D printing system that enables rapid production of large parts. The density of the printed magnet is ∼ 5.2 g/cm3. The room temperature magnetic properties are: intrinsic coercivity Hci = 8.9 kOe (708.2 kA/m), remanence Br = 5.8 kG (0.58 T), and energy product (BH)max = 7.3 MGOe (58.1 kJ/m3). The as-printed magnets are then coated with two types of polymers, both of which improve the thermal stability as revealed by flux aging loss measurements. Tensile tests performed at 25 °C and 100 °C show that the ultimate tensile stress (UTS) increases with increasing loading fraction of the magnet powder, and decreases with increasing temperature. AC magnetic susceptibility and resistivity measurements show that the 3D printed Nd-Fe-B bonded magnets exhibit extremely low eddy current loss and high resistivity. Finally, we demonstrate the performance of the 3D printed magnets in a DC motor configuration via back electromotive force measurements.

Anisotropic bonded Nd2Fe14B (NdFeB) magnets in a polycarbonate (PC) binder matrix are fabricated using a compression molding process. The weight fractions (w.f.) of NdFeB in PC on the batch mixer are 20, 50, 75, 85 and 95% compared to the twin screw extruder with 20, 50 and 75% respectively. The density of the 95% batch mixed magnets fabricated was 5.34 g/cm3 and the magnetic properties are, intrinsic coercivity Hci = 942.99 kA/m, remanence Br = 0.86 T, and energy product (BH)max = 120.96 kJ/m3. The measured tensile properties are in the range of 27-59 MPa, comparable to that of polyamide (PA), polyphenylene sulfide (PPS) bonded magnets and demonstrating potential for bonded magnet applications. Scanning electron microscopy showed that the onset of failure occurs in the magnetic particle- matrix interface. This study demonstrates that compression additive molding technique can be used to fabricate high performance NdFeB polycarbonate composite magnets with improved mechanical properties.

A multifunctional device produces a much-improved thermoelectric-driven transverse voltage by exploiting a thermoelectric current to drive an anomalous Hall effect in a ferromagnet.

Advances in crystal growth have allowed for synthesis of large single crystals of Nd 1 + ∊ Fe 4 B 4 , a well-known phase with a modulated structure. As a result we are able to report heat capacity and resistivity measurements on a single crystal Nd 1 + ∊ Fe 4 B 4 sample with a distribution of ∊ that skews towards the solubility limit of Nd near ∊ ≈ 1 7 . Heat capacity measurements show evidence of crystal field splitting at temperatures higher than the long-range ferromagnetic Curie temperature. Heat capacity, resistivity, and magnetization measurements all confirm a Curie temperature of 7 K which is lower than previously reported values in the Nd 1 + ∊ Fe 4 B 4 system. We also perform measurements of the angular dependence of the magnetization and discover behavior associated with the magnetic anisotropy that is inconsistent with the simple description previously proposed.

Single crystals of ( Nd 1 − x Ce x ) 2 Fe 14 B , some reaching ∼ 6 × 8 × 8 mm 3 in volume, are grown out of Fe-(Nd, Ce) flux. This crystal growth method allows for large ( Nd 1 − x Ce x ) 2 Fe 14 B single crystals to be synthesized using a simple flux growth procedure. Chemical and structural analyses of the crystals indicate that ( Nd 1 − x Ce x ) 2 Fe 14 B forms a solid solution until at least x =0.38 with a Vegard-like variation of the lattice constants with x . Refinements of single crystal neutron diffraction data indicate that Ce has a slight site preference (7:3) for the 4 g rare earth site over the 4 f site. Magnetization measurements at 300 K show only small decreases with increasing Ce content in saturation magnetization ( M s ) and anisotropy field ( H A ), and Curie temperature ( T C ). First principles calculations are carried out to understand the effect of Ce substitution on the electronic and magnetic properties. For a multitude of applications, it is expected that the advantage of incorporating lower-cost and more abundant Ce will outweigh the small adverse effects on magnetic properties. Ce-substituted Nd 2 Fe 14 B is therefore a potential high-performance permanent magnet material with substantially reduced Nd content.

The phase formation behavior of the nominal CeFe 8 Co 3 Ti 1 − y Si y system is investigated for 0 ≤ y ≤ 0.6 by powder x-ray diffraction and scanning electron microscopy with energy dispersive x-ray spectroscopy for ingots formed by arc-melting then annealing at 1000 °C and quenching to room temperature. The ingots are seen to nearly single phase for y ≤ 0.4 and are multi-phase for y ≥ 0.5 though a compound of the ThMn 12 type does indeed form for all values of y . The saturation magnetizations ( M s ), Curie temperatures ( T C ), and magnetic anisotropy fields ( H a ) are measured for the y ≤ 0.4 samples and the values of M s and H a appear to be nearly identical for all y ≤ 0.4 . T C , however, is seen to increase about 20 °C in this range for increasing y .

In the present work we examine the intrinsic magnetic and structural properties of the title alloys, permanent magnet materials based on the abundant rare-earth elements lanthanum and cerium, since these properties ( T C , M s H a ( K 1 , K 2 )) will set the upper limits on the quality of permanent magnet that can be fabricated from said alloys. Ce 2 Co 16 Ti has a high magnetic anisotropy ( H a = 65 kOe) but a relatively low saturation magnetization ( M s = 7.3 kG), and La 2 Co 16 Ti has a high M s (9.5 kG) but H a too low for most applications (16 kOe). Though these two end-members have previously well-known properties, changing economic conditions have made re-examination of systems containing cerium and lanthanum necessary as the economic viability of rare earth mining becomes dependent on extraction of products beyond what is currently considered useful and profitable within the rare earth elements. We find that replacing some lanthanum with cerium in La 2 Co 16 Ti increases H a by a factor of more than two, while decreasing M s by less than 5%. The measured M s indicate maximum possible energy products in excess of 20 MG·Oe in these materials, which have Curie temperatures near 600 °C. Real energy products are expected to be greatest near x = 1. These findings identify La x Ce 2−x Co 16 Ti as a promising system for development of so-called gap magnets that fill the energy product gap between expensive rare-earth magnets and current non-rare earth alternatives.

Configurational disorder can have a dominating role in the formation of macroscopic functional responses in strongly correlated materials. Here, we use entropy-stabilization synthesis to create single-crystal epitaxial $\mathrm{AB}{\mathrm{O}}_{3}$ perovskite thin films with equal atomic concentration of 3d transition-metal cations on the B-site sublattice. X-ray diffraction, atomic force microscopy, and scanning transmission electron microscopy of $\mathrm{La}(\mathrm{C}{\mathrm{r}}_{0.2}\mathrm{M}{\mathrm{n}}_{0.2}\mathrm{F}{\mathrm{e}}_{0.2}\mathrm{C}{\mathrm{o}}_{0.2}\mathrm{N}{\mathrm{i}}_{0.2}){\mathrm{O}}_{3}$ (L5BO) films demonstrate excellent crystallinity, smooth film surfaces, and uniform mixing of the 3d transition-metal cations throughout the B-site sublattice. The magnetic properties are strongly dependent on substrate-induced lattice anisotropy and suggest the presence of long-range magnetic order in these exceptionally disordered materials. The ability to populate multiple elements onto a single sublattice in complex crystal structures opens new possibilities to design functionality in correlated systems and enable novel fundamental studies seeking to understand how diverse local bonding environments can work to generate macroscopic responses, such as those driven by electron-phonon channels and complex exchange interaction pathways.

Single crystals of the single kagome layer compound FeSn are investigated using x-ray and neutron scattering, magnetic susceptibility and magnetization, heat capacity, resistivity, Hall, Seebeck, thermal expansion, thermal conductivity measurements, and density functional theory (DFT). FeSn is a planar antiferromagnet below ${T}_{\mathrm{N}}=365\phantom{\rule{0.28em}{0ex}}\mathrm{K}$ and exhibits ferromagnetic magnetic order within each kagome layer. The in-plane magnetic susceptibility is sensitive to synthesis conditions. Resistivity, Hall and Seebeck results indicate multiple bands near the Fermi energy. The resistivity of FeSn is \ensuremath{\approx}3 times lower for current along the stacking direction than in the plane, suggesting that transport and the bulk electronic structure of FeSn is not quasi-two-dimensional (2D). FeSn is an excellent metal with \ensuremath{\rho}(300 K)/\ensuremath{\rho}(2 K) values \ensuremath{\approx}100 in both directions. While the ordered state is antiferromagnetic, high temperature susceptibility measurements indicate a ferromagnetic Curie-Weiss temperature of 173 K, reflecting the strong in-plane ferromagnetic interactions. DFT calculations show a 3D electronic structure with the Dirac nodal lines along the K-H directions in the magnetic Brillouin zone about 0.3 eV below the Fermi energy, with the Dirac dispersions at the $K$ points gapped by spin-orbit coupling except at the $H$ point. The magnetism, however, is highly 2D with ${J}_{\mathrm{in}\text{\ensuremath{-}}\mathrm{plane}}/{J}_{\mathrm{out}\text{\ensuremath{-}}\mathrm{of}\text{\ensuremath{-}}\mathrm{plane}}\ensuremath{\approx}10$. The predicted spin-wave spectrum is presented.

FeSn is an itinerant antiferromagnet that hosts electronic Dirac states and ordered magnetic moments lying within its Fe Kagome-lattice planes. We present magnetization measurements of single crystals of $({\mathrm{Fe}}_{1\ensuremath{-}x}{\mathrm{Co}}_{x})\text{Sn}$, revealing the evolution and suppression of this magnetic order with Co substitution. We interpret the dramatic changes in magnetic anisotropy to indicate a reorientation of the moments from perpendicular to parallel to the hexagonal $c$ axis and confirm this with neutron diffraction. It has been proposed that the Dirac nodes observed in FeSn should become gapped if the moments rotate as our data suggests. We identify Co-substituted compositions that adopt both antiferromagnetic configurations at different temperatures. This system provides a unique opportunity to study how the details of magnetic order impact Dirac electron states.

Here, the authors report a thorough study of the evolution of structural, magnetic, and electrical properties of MnBi${}_{2\ensuremath{-}x}$Sb${}_{x}$Te${}_{4}$ single crystals. This investigation reveals an intimate correlation between the structural, magnetic, and transport properties. Partial substitution of Bi by Sb is an effective approach to tuning both the magnetism and the Fermi level, which are two key components of magnetic topological insulators. This work provides an important guide for exploring the topological properties in MnBi${}_{2}$Te${}_{4}$-based materials. The effect of doping on the magnetic properties also suggests complex competing interactions, which should be considered when tuning the magnetic properties.

Most interesting examples of violations of the Mott-Ioffe-Regel (MIR) resistivity limit are found in materials with strong electronic correlations that are not well understood by theory. We demonstrate that first principles theory can predict the experimentally observed frequency dependence of the optical conductivity for a novel class of metals where the residual resistivity is near or above the MIR limit, which we define as a ``bad metal.'' The predicted optical conductivity of a NiCoCr alloy is in good agreement with experiment. It is demonstrated that the width of the Drude peak describing the low-frequency part of optical conductivity is comparable to the Fermi energy. The latter, together with a mean free path comparable to the interatomic distance, indicates the absence of well-defined quasiparticles. In contrast to traditional bad metals with strong electron-electron interactions, both the high resistivity and the large width of the Drude peak in these alloys result from strong scattering on disordered atomic potentials that can be understood using modern density functionals.

Single crystals of the van der Waals layered $5d$ transition-metal compound ${\mathrm{Os}}_{0.55}{\mathrm{Cl}}_{2}$ were grown and characterized by x-ray diffraction, magnetization and heat-capacity measurements, and atomic resolution electron microscopy. The crystals are stable in air and easily cleaved. The structure is derived from the ${\mathrm{CdCl}}_{2}$ structure type, with triangular layers of transition metal sites coordinated by edge-sharing octahedra of Cl and separated by a van der Waals gap. On average, only 55% of the metal sites are occupied by Os, and evidence for short- and long-ranged vacancy orders is observed by diffraction and real-space imaging. Magnetization data indicate magnetocrystalline anisotropy due to spin-orbit coupling, antiferromagnetic correlations, and no sign of magnetic order or spin freezing down to 0.4 K. Heat-capacity measurements in applied magnetic fields show only a broad, field-dependent anomaly. The magnetic susceptibility and heat capacity obey power laws at low temperature and low field with exponents close to 0.5. The power law behaviors of the low-temperature heat capacity and magnetic susceptibility suggest gapless magnetic fluctuations prevent spin freezing or ordering in ${\mathrm{Os}}_{0.55}{\mathrm{Cl}}_{2}$. Divergence of the magnetic Gruneisen parameter indicates nearness to a magnetic quantum critical point. Similarities to behaviors of spin-liquid materials are noted, and in total the results suggest ${\mathrm{Os}}_{0.55}{\mathrm{Cl}}_{2}$ may be an example of a quantum spin liquid in the limit of strong chemical disorder.

Lead chalcogenides have exceptional thermoelectric properties and intriguing anharmonic lattice dynamics underlying their low thermal conductivities. An ideal material for thermoelectric efficiency is the phonon glass–electron crystal, which drives research on strategies to scatter or localize phonons while minimally disrupting electronic-transport. Anharmonicity can potentially do both, even in perfect crystals, and simulations suggest that PbSe is anharmonic enough to support intrinsic localized modes that halt transport. Here, we experimentally observe high-temperature localization in PbSe using neutron scattering but find that localization is not limited to isolated modes – zero group velocity develops for a significant section of the transverse optic phonon on heating above a transition in the anharmonic dynamics. Arrest of the optic phonon propagation coincides with unusual sharpening of the longitudinal acoustic mode due to a loss of phase space for scattering. Our study shows how nonlinear physics beyond conventional anharmonic perturbations can fundamentally alter vibrational transport properties., To optimize the performance of lead chalcogenides for thermoelectric applications, strategies to further reduce the crystal’s thermal conductivity is required. Here, the authors discover anharmonic localized vibrations in PbSe crystals for optimizing the crystal’s vibrational transport properties.

Author(s): Vilmercati, P; Kim, Y; Mo, SK; McGuire, M; Sales, B; Mandrus, D; Ku, W; Sangaletti, L; Singh, DJ; Mannella, N | Abstract: We report systematic temperature- and doping-dependent measurements of the Fe3s core-level photoemission spectra in the normal state of superconducting Sr(Fe1-xCox)2As2. The analysis of the Fe3s spectrum provides an element-specific determination of the mean value of the magnitude of the Fe spin moment measured on the fast (10-16-10-15s) timescale of the photoemission process. The data reveal the ubiquitous presence in the normal state of Fe spin moments with magnitude fluctuating on short timescales. The data reveal a significant reduction of the magnitude of the effective Fe spin moment on going from the parent to the optimal doped compound. The doping dependence of the magnitude of the spin moment at higher doping level is less clear, being either constant, or even nonmonotonic, depending on temperature. This phenomenology indicates the importance of the interaction between spin and itinerant degrees of freedom in shaping the properties of the normal state. These findings reaffirm the complexity of the normal state of 122 Fe-pnictides, which are typically viewed as the least correlated of the high-temperature unconventional superconductors.

The coexistence and competition between superconductivity and electronic orders, such as spin or charge density waves, have been a central issue in high transition-temperature (${T_{\rm c}}$) superconductors. Unlike other iron-based superconductors, FeSe exhibits nematic ordering without magnetism whose relationship with its superconductivity remains unclear. More importantly, a pressure-induced fourfold increase of ${T_{\rm c}}$ has been reported, which poses a profound mystery. Here we report high-pressure magnetotransport measurements in FeSe up to $\sim9$ GPa, which uncover a hidden magnetic dome superseding the nematic order. Above ${\sim6}$ GPa the sudden enhancement of superconductivity (${T_{\rm c}\le38.3}$ K) accompanies a suppression of magnetic order, demonstrating their competing nature with very similar energy scales. Above the magnetic dome we find anomalous transport properties suggesting a possible pseudogap formation, whereas linear-in-temperature resistivity is observed above the high-${T_{\rm c}}$ phase. The obtained phase diagram highlights unique features among iron-based superconductors, but bears some resemblance to that of high-${T_{\rm c}}$ cuprates., Comment: 15 pages, 4 figures

The interactions between electrons and lattice vibrations are fundamental to materials behaviour. In the case of group IV–VI, V and related materials, these interactions are strong, and the materials exist near electronic and structural phase transitions. The prototypical example is PbTe whose incipient ferroelectric behaviour has been recently associated with large phonon anharmonicity and thermoelectricity. Here we show that it is primarily electron-phonon coupling involving electron states near the band edges that leads to the ferroelectric instability in PbTe. Using a combination of nonequilibrium lattice dynamics measurements and first principles calculations, we find that photoexcitation reduces the Peierls-like electronic instability and reinforces the paraelectric state. This weakens the long-range forces along the cubic direction tied to resonant bonding and low lattice thermal conductivity. Our results demonstrate how free-electron-laser-based ultrafast X-ray scattering can be utilized to shed light on the microscopic mechanisms that determine materials properties., Group IV–VI materials often exist in a state near an electronic or structural phase transition. Here, the authors use ultrafast X-ray scattering to show that coupling of band-edge electrons and phonons causes the ferroelectric instability observed in lead telluride.

Extrusion based additive manufacturing of polymer composite magnets can increase the solid loading volume fraction with greater mechanical force through the printing nozzle as compared to traditional injection molding process. About 63 vol% of isotropic NdFeB magnet powders were compounded with 37 vol% of polyphenylene sulfide and bonded permanent magnets were fabricated while using Big Area Additive Manufacturing without any degradation in magnetic properties. The polyphenylene sulfide bonded magnets have a tensile stress of 20 MPa, almost double than that of nylon bonded permanent magnets. Additively manufactured and surface-protective-resin coated bonded magnets meet the industrial stability criterion of up to 175 °C with a flux-loss of 2.35% over 1000 h. They also exhibit better corrosion resistance behavior when exposed to acidic (pH = 1.35) solution for 24 h and also annealed at 80 °C over 100 h (at 95% relative humidity) over without coated magnets. Thus, polyphenylene sulfide bonded, additively manufactured, protective resin coated bonded permanent magnets provide better thermal, mechanical, and magnetic properties.

Oxygen interstitials and vacancies play a key role in modulating the microstructure and properties of nonstoichiometric oxide systems, such as those used for superconductors and multiferroics. Key to understanding the tuning mechanisms resulting from oxygen doping is a knowledge of the precise positions of these lattice defects, and of the interaction both between these defects and with many order parameters. Here, we report how such information can, for the first time, be obtained from a sample of ${\mathrm{LuFe}}_{2}{\mathrm{O}}_{4.22}$ using a range of techniques including advanced electron microscopy, atomic-resolution spectroscopy, and density functional theory calculations. The results provide quantitative atomic details of the crystal unit cell, together with a description of the ferroelastic, ferroelectric, and ferromagnetic order parameters. We elucidate also the interaction between these order parameters and the positions of the oxygen interstitials in the oxygen-enriched sample. The comprehensive analysis of oxygen interstitial ordering provides insights into understanding the coupling among different degrees of freedom in rare earth ferrites and demonstrates that oxygen content regulation is a powerful tool for tuning the microstructure and properties for this class of quantum material.

Electronic phase separation has been increasingly recognized as an important phenomenon in understanding many of the intriguing properties displayed in transition metal oxides. It is believed to produce fascinating functional properties in otherwise chemically homogenous electronic systems, e.g., colossal magnetoresistance manganites and high-${T}_{\mathrm{c}}$ cuprates. While many well-known electronically phase-separated systems are oxides, it has been argued that the same phenomenon should occur in other electronic systems with strong competing interactions. Here we report the observation of electronic phase separation in molecular $({\mathrm{ND}}_{4}{)}_{2}{\mathrm{FeCl}}_{5}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathrm{D}}_{2}\mathrm{O}$, a type-II multiferroic. We show that two magnetic phases, one of which is commensurate and the other of which is incommensurate, coexist in this material. Their evolution under applied magnetic field produces emergent properties. In particular, our measurements reveal a field-induced exotic state linked to a direct transition from a paraelectric/paramagnetic phase to a ferroelectric/antiferromagnetic phase, a collective phenomenon that hasn't been seen in other magnetic multiferroics.

Two-dimensional $\ensuremath{\beta}\text{\ensuremath{-}}{\mathrm{MoCl}}_{4}$ is an attractive material from the perspectives of magnetism in $4d$ transition metal compounds, geometrically frustrated lattices, and magnetic van der Waals layered materials, but the magnetism in this compound has not been particularly well studied to date. Here the magnetic properties and crystal structure of ${\mathrm{MoCl}}_{4}$ are revisited, and results of ac and dc magnetic measurements and single crystal x-ray diffraction are reported. Crystals grow as well-formed and easily cleaved hexagonal plates that are unstable in air. The revised structural model comprises ${\mathrm{CdCl}}_{2}$-type layers with 50% Mo vacancies distributed over the sites of the triangular cation net. Interestingly, a structural ambiguity regarding the vacancy distribution is identified in the analysis of the diffraction data. The orbital moment is not expected to be quenched in this $4{d}^{2}$ compound. Accordingly, magnetization measurements indicate an effective moment that is about 20% lower than the spin-only value. The magnetic data reveal an anomaly near 5 K, below which a divergence of field-cooled and zero-field-cooled dc magnetization, a slow relaxation of thermoremanent magnetization, and enhanced frequency dependence of ac magnetization are observed. Thus, $\ensuremath{\beta}\text{\ensuremath{-}}{\mathrm{MoCl}}_{4}$ represents an uncommon example of a cleavable spin-glass system.

BAs was predicted to have an unusually high thermal conductivity at room temperature of 2000$\,$Wm$^{-1}$$\,$K$^{-1}$, comparable to that of diamond. However, the experimentally measured thermal conductivity of BAs single crystals is an order of magnitude lower. To identify the origin of this large inconsistency, we investigated the lattice structure and potential defects in BAs single crystals at atomic scale using aberration-corrected scanning transmission electron microscopy (STEM). Rather than finding a large concentration As vacancies ($V_\mathrm{As}$), as widely thought to dominate the thermal resistance in BAs crystals, our STEM results showed enhanced intensity of some B columns and reduced intensity of some As columns, suggesting the presence of antisite defects with As$_\mathrm{B}$ (As-atom on B site) and B$_\mathrm{As}$ (B-atom on As site) with significant concentrations. Further calculations show that the antisite pair with As$_\mathrm{B}$ next to B$_\mathrm{As}$ is preferred energetically among the different types of point defects investigated, and confirm that such defects lower the thermal conductivity for BAs. Using a concentration of 6.6$\pm$3$\times$10$^{20}$$\,$cm$^{-3}$ for the antisite pairs estimated from STEM images, thermal conductivity is estimated to be 65-100$\,$Wm$^{-1}$$\,$K$^{-1}$, in reasonable agreement with our measured value. Our study suggests that As$_\mathrm{B}$-B$_\mathrm{As}$ antisite pairs are the primary lattice defects suppressing thermal conductivity of BAs. Possible approaches are proposed for growth of high quality crystals or films with high thermal conductivity., Comment: 4 pages and 3 figures in main text; 4 pages and 4 figures in the Supplementary Material