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The theory of bulk orbital magnetization has been formulated both in reciprocal space based on Berry curvature and related quantities, and in real space in terms of the spatial average of a quantum mechanical local marker. Here we consider a three-dimensional antiferromagnetic material having a vanishing bulk but a nonzero surface orbital magnetization. We ask whether the surface-normal component of the surface magnetization is well defined, and if so, how to compute it. As the physical observable corresponding to this quantity, we identify the macroscopic current running along a hinge shared by two facets. However, the hinge current only constrains the difference of the surface magnetizations on the adjoined facets, leaving a potential ambiguity. By performing a symmetry analysis, we find that only crystals exhibiting a pseudoscalar symmetry admit well-defined magnetizations at their surfaces at the classical level. We then explore the possibility of computing surface magnetization via a coarse-graining procedure applied to a quantum local marker. We show that multiple expressions for the local marker exist, and apply constraints to filter out potentially meaningful candidates. Using several tight-binding models as our theoretical test bed and several potential markers, we compute surface magnetizations for slab geometries and compare their predictions with explicit calculations of the macroscopic hinge currents of rod geometries. We find that only a particular form of the marker consistently predicts the correct hinge currents., 26 pages, 12 figures

The Su, Schrieffer and Heeger (SSH) model, describing the soliton excitations in polyacetylene due to the formation of antiphase domain walls (DW) from the alternating bond pattern, has served as a paradigmatic example of one-dimensional (1D) chiral topological insulators. While the SSH model has been realized in photonic and plasmonic systems, there have been limited analogues in three-dimensional (3D) electronic systems, especially regarding the formation of antiphase DWs. Here, we propose that pristine bulk Bi, in which the dimerization of $(111)$ atomic layers renders alternating covalent and van der Waals bonding within and between successive $(111)$ bilayers, respectively, serves as a 3D analogue of the SSH model. First, we confirm that the two dimerized Bi structures belong to different Zak phases of 0 and $\pi$ by considering the parity eigenvalues and Wannier charge centers, while the previously reported bulk topological phases of Bi remain invariant under the dimerization reversal. Next, we demonstrate the existence of topologically non-trivial $(111)$ and trivial $(11\bar{2})$ DWs in which the number of in-gap DW states (ignoring spin) is odd and even respectively, and show how this controls the interlinking of the Zak phases of the two adjacent domains. Finally, we derive general criteria specifying when a DW of arbitrary orientation exhibits a $\pi$ Zak phase based on the flip of parity eigenvalues. An experimental realization of dimerization in Bi and the formation of DWs may be achieved via intense femtosecond laser excitations that can alter the interatomic forces and bond lengths.

Emergent relativistic quasiparticles in Weyl semimetals are the source of exotic electronic properties such as surface Fermi arcs, the anomalous Hall effect and negative magnetoresistance, all observed in real materials. Whereas these phenomena highlight the effect of Weyl fermions on the electronic transport properties, less is known about what collective phenomena they may support. Here, we report a Weyl semimetal, NdAlSi, that offers an example. Using neutron diffraction, we found a long-wavelength helical magnetic order in NdAlSi, the periodicity of which is linked to the nesting vector between two topologically non-trivial Fermi pockets, which we characterize using density functional theory and quantum oscillation measurements. We further show the chiral transverse component of the spin structure is promoted by bond-oriented Dzyaloshinskii–Moriya interactions associated with Weyl exchange processes. Our work provides a rare example of Weyl fermions driving collective magnetism. The Weyl fermions in NdAlSi mediate a helical incommensurate spin density wave, providing a rare example of Weyl-mediated collective phenomena.

We report direct visualization of spin-flip transition of the surface layer in antiferromagnet MnBi_{4}Te_{7}, a natural superlattice of alternating MnBi_{2}Te_{4} and Bi_{2}Te_{3} layers, using cryogenic magnetic force microscopy (MFM). The observation of magnetic contrast across domain walls and step edges confirms that the antiferromagnetic order persists to the surface layers. The magnetic field dependence of the MFM images reveals that the surface magnetic layer undergoes a first-order spin-flip transition at a magnetic field that is lower than the bulk transition, in excellent agreement with a revised Mills model. Our analysis suggests no reduction of the order parameter in the surface magnetic layer, implying robust ferromagnetism in the single-layer limit. The direct visualization of surface spin-flip transition not only opens up exploration of surface metamagnetic transitions in layered antiferromagnets, but also provides experimental support for realizing quantized transport in ultrathin films of MnBi_{4}Te_{7} and other natural superlattice topological magnets.

The Joint Automated Repository for Various Integrated Simulations (JARVIS) is an integrated infrastructure to accelerate materials discovery and design using density functional theory (DFT), classical force-fields (FF), and machine learning (ML) techniques. JARVIS is motivated by the Materials Genome Initiative (MGI) principles of developing open-access databases and tools to reduce the cost and development time of materials discovery, optimization, and deployment. The major features of JARVIS are: JARVIS-DFT, JARVIS-FF, JARVIS-ML, and JARVIS-tools. To date, JARVIS consists of ≈40,000 materials and ≈1 million calculated properties in JARVIS-DFT, ≈500 materials and ≈110 force-fields in JARVIS-FF, and ≈25 ML models for material-property predictions in JARVIS-ML, all of which are continuously expanding. JARVIS-tools provides scripts and workflows for running and analyzing various simulations. We compare our computational data to experiments or high-fidelity computational methods wherever applicable to evaluate error/uncertainty in predictions. In addition to the existing workflows, the infrastructure can support a wide variety of other technologically important applications as part of the data-driven materials design paradigm. The JARVIS datasets and tools are publicly available at the website: https://jarvis.nist.gov.

van der Waals materials are exceptionally responsive to external stimuli. Pressure-induced layer sliding, metallicity, and superconductivity are fascinating examples. Inspired by opportunities in this area, we combined high-pressure optical spectroscopies and first-principles calculations to reveal piezochromism in MnPS3. Dramatic color changes (green → yellow → red → black) take place as the charge gap shifts across the visible regime and into the near infrared, moving systematically toward closure at a rate of approximately −50 meV/GPa. This effect is quenched by the appearance of the insulator–metal transition. In addition to uncovering an intriguing and tunable functionality that is likely to appear in other complex chalcogenides, the discovery that piezochromism can be deterministically controlled at room temperature accelerates the development of technologies that take advantage of stress-activated modification of electronic structure.

The layered metal phosphorous trisulfide FePS$_3$ is reported to be a Mott insulator at ambient conditions and to undergo structural and insulator-metal phase transitions under pressure. However, the character of the resulting metallic states has not been understood clearly so far. Here, we theoretically study the phase transitions of FePS$_3$ using first-principles methods based on density functional theory and embedded dynamical mean field theory. We find that the Mott transition in FePS$_3$ can be orbital-selective, with $t_{2g}$ states undergoing a correlation-induced insulator-to-metal transition while $e_g$ states remain gapped. We show that this orbital-selective Mott phase, which occurs only when non-hydrostatic pressure is used, is a bad metal (or non-Fermi liquid) with large fluctuating moments due to Hund's coupling. Further application of pressure increases the crystal-field splitting and converts the system to a conventional Fermi liquid with low-spin configurations dominant. Our results show that FePS$_3$ is a novel example of a system that realizes an orbital-selective Mott phase, allowing tuning between correlated and uncorrelated metallic properties in an accessible pressure range ($\leq$ 18 GPa)., 5 pages, 5 figures

The group-IV diamond-structure elements are known to host a variety of planar defects, including {001} planar defects in C and {001}, {111} and {113} planar defects in Si and Ge. Among the {001} planar defects, the Humble defect, known for some time to occur in Ge, has recently also been observed in Si/Ge alloys, but the details of its electronic structure remain poorly understood. Here we perform first-principles density functional calculations to study Humble defects in both Ge and Ge$_{0.8}$Si$_{0.2}$. We also measure the Si L$_{2,3}$-edge electron energy loss spectra both at the defect and in a bulk-like region far from the defect, and compare with theoretical calculations on corresponding Si sites in our first-principles calculations. We find that inclusion of core-hole effects in the theory is essential for reproducing the observed L$_{2,3}$ edge spectra, and that once they are included, the results provide a set of fingerprints for different types of local atomic bonding environments in Ge$_{0.8}$Si$_{0.2}$. Our first-principles calculations reveal that the Humble defects have a tendency to enlarge the electronic band gap, which may have potential uses in band engineering. The use of hybrid functionals for an improved description of the band gap in these systems is also discussed., Comment: 11 pages, 10 figures; Comments are welcome

We report a new \{001\} planar defect found in SiGe nanopillars. The defect structure, determined by atomic resolution electron microscopy, matches the Humble defect model proposed for diamond. We also investigated several possible variants of the Humble structure using first principles calculations and found that the one lowest in energy was also in best agreement with the STEM images. The pillar composition has been analyzed with electron energy loss spectroscopy, which hints at how the defect is formed. Our results show that the structure and formation process of defects in nanostructured group IV semiconductors can be different from their bulk counterparts.

Orientation dependent electronic properties of wurtzite zinc oxide nanorods are characterized by aloof beam electron energy-loss spectroscopy (EELS) carried out in a scanning transmission electron microscope (STEM). The two key crystal orientation differentiating transitions specific to the in-plane (13.0 eV) and out-of-plane (11.2 eV) directions with respect to the wurtzite structure are examined by first principles density-functional theory calculations. We note some degree of orientation dependence at the onset of direct band gap transition near 3.4 eV. We demonstrate that good polarization selectivity can be achieved by placing the electron probe at different locations around the specimen with increasing impact parameter while keeping the beam-specimen orientation fixed. The observed results are qualitatively elucidated in terms of the perpendicular electric fields generated by the fast electron (60 kV) used in the microscope. The fact that good polarization selectivity can be achieved by aloof beam EELS without the requirement of sample reorientation is an attractive aspect from the characterization method point of view in the STEM-EELS community., 9 pages and 9 figures

We explore dynamic interactions between the crystal lattice and magnetic degrees of freedom in a frustrated magnetic system using the example of a pyrochlore quantum spin-ice candidate ${\mathrm{Pr}}_{2}{\mathrm{Zr}}_{2}{\mathrm{O}}_{7}$. Using Raman scattering spectroscopy we demonstrate that crystal electric field excitations of Pr3+, which define the magnetic properties of ${\mathrm{Pr}}_{2}{\mathrm{Zr}}_{2}{\mathrm{O}}_{7}$, cannot be understood within a model of a static lattice. We identify vibronic interactions with a phonon which lead to a splitting of a doublet crystal field excitation at around 55 meV. We also observe an unconventional behavior of a splitting of the non-Kramers ground state doublet of ${\mathrm{Pr}}^{3+}$, revealed by observing excitations to the first excited singlet state ${E}_{g}^{0}\ensuremath{\rightarrow}{A}_{1g}$ at around 10 meV. The splitting has a strong temperature dependence, where the doublet structure is most prominent between 50 and 100 K, and the weight of one of the components strongly decreases on cooling contrary to simple thermal population tendency. We suggest a static or dynamic deviation of ${\mathrm{Pr}}^{3+}$ from the position in the ideal crystal structure can be the origin of the effect, with the deviation strongly decreasing at low temperatures.

${\mathrm{GeCo}}_{2}{\mathrm{O}}_{4}$ is a unique system in the family of cobalt spinels $A{\mathrm{Co}}_{2}{\mathrm{O}}_{4}$ ($A$= Sn, Ti, Ru, Mn, Al, Zn, Fe, etc.) in which magnetic Co ions stabilize on the pyrochlore lattice exhibiting a large degree of orbital frustration. Due to the complexity of the low-temperature antiferromagnetic (AFM) ordering and long-range magnetic exchange interactions, the lattice dynamics and magnetic structure of a ${\mathrm{GeCo}}_{2}{\mathrm{O}}_{4}$ spinel have remained puzzling. To address this issue, here we present theoretical and experimental investigations of the highly frustrated magnetic structure, and the infrared (IR) and Raman-active phonon modes in the spinel ${\mathrm{GeCo}}_{2}{\mathrm{O}}_{4}$, which exhibits an AFM ordering below the N\'eel temperature ${T}_{N}\ensuremath{\sim}21$ K and an associated cubic ($Fd\overline{3}m$) to tetragonal ($I{4}_{1}/amd$) structural phase transition whose location at ${T}_{N}$ vs at a lower ${T}_{S}\ensuremath{\sim}16$ K is controversial. Our density functional theory ($\mathrm{DFT}+U$) calculations reveal that one needs to consider magnetic-exchange interactions up to the third-nearest neighbors to get an accurate description of the low-temperature AFM order in ${\mathrm{GeCo}}_{2}{\mathrm{O}}_{4}$. At room temperature, three distinct IR-active modes (${T}_{1\mathrm{u}}$) are observed at frequencies 680, 413, and 325 ${\mathrm{cm}}^{\ensuremath{-}1}$ along with four Raman-active modes ${A}_{1\mathrm{g}}, {T}_{2\mathrm{g}}$(1), ${T}_{2\mathrm{g}}$(2), and ${E}_{\mathrm{g}}$ at frequencies 760, 647, 550, and 308 ${\mathrm{cm}}^{\ensuremath{-}1}$, respectively, which match reasonably well with our $\mathrm{DFT}+U$ calculated values. All the IR-active and Raman-active phonon modes exhibit signatures of moderate spin-phonon coupling. The temperature dependence of various parameters, such as the shift, width, and intensity, of the Raman-active modes is also discussed. Noticeable changes around ${T}_{N}\ensuremath{\sim}21$ K and ${T}_{S}\phantom{\rule{4pt}{0ex}}\ensuremath{\sim}16$ K are observed in the Raman line parameters of the ${E}_{\mathrm{g}}$ and ${T}_{2\mathrm{g}}$(1) modes, which are associated with the modulation of the Co-O bonds in ${\mathrm{CoO}}_{6}$ octahedra during the excitations of these modes.

Various methods going beyond density functional theory (DFT), such as DFT+U, hybrid functionals, meta-GGAs, GW, and DFT-embedded dynamical mean field theory (eDMFT), have been developed to describe the electronic structure of correlated materials, but it is unclear how accurate these methods can be expected to be when applied to a given strongly correlated solid. It is thus of pressing interest to compare their accuracy as they apply to different categories of materials. Here we introduce a novel paradigm in which a chosen set of beyond-DFT methods is systematically and uniformly tested on a chosen class of materials. For a first application, we choose the target materials to be the binary transition metal oxides FeO, CoO, MnO, and NiO in their antiferromagnetic phase and present a head-to-head comparison of spectral properties as computed using the various methods. We also compare with available experimental angle-resolved photoemission spectroscopy (ARPES), inverse-photoemission spectroscopy, and with optical absorption. For the class of compounds studied here, we find that both B3LYP and eDMFT reproduce the experiments quite well, with eDMFT doing best, in particular when comparing with the ARPES data.

Much of the dramatic growth in research on topological materials has focused on topologically protected surface states. While the domain walls of topological materials such as Weyl semimetals with broken inversion or time-reversal symmetry can provide a hunting ground for exploring topological interfacial states, such investigations have received little attention to date. Here, utilizing in-situ cryogenic transmission electron microscopy combined with first-principles calculations, we discover intriguing domain-wall structures in MoTe2, both between polar variants of the low-temperature(T) Weyl phase, and between this and the high-T high-order topological phase. We demonstrate how polar domain walls can be manipulated with electron beams and show that phase domain walls tend to form superlattice-like structures along the c axis. Scanning tunneling microscopy indicates a possible signature of a conducting hinge state at phase domain walls. Our results open avenues for investigating topological interfacial states and unveiling multifunctional aspects of domain walls in topological materials., 6 figures

The topology of electronic states in band insulators with mirror symmetry can be classified in two different ways. One is in terms of the mirror Chern number, an integer that counts the number of protected Dirac cones in the Brillouin zone of high-symmetry surfaces. The other is via a Z2 index that distinguishes between systems that have a nonzero quantized orbital magnetoelectric coupling (“axion-odd”), and those that do not (“axion-even”); this classification can also be induced by other symmetries in the magnetic point group, including time reversal and inversion. A systematic characterization of the axion Z2 topology has previously been obtained by representing the valence states in terms of hybrid Wannier functions localized along one chosen crystallographic direction, and inspecting the associated Wannier band structure. Here we focus on mirror symmetry, and extend that characterization to the mirror Chern number. We choose the direction orthogonal to the mirror plane as the Wannierization direction and show that the mirror Chern number can be determined from the winding numbers of the touching points between Wannier bands on mirror-invariant planes and from the Chern numbers of flat bands pinned to those planes. In this representation, the relation between the mirror Chern number and the axion Z2 index is readily established. The formalism is illustrated by means of ab initio calculations for SnTe in the monolayer and bulk forms, complemented by tight-binding calculations for a toy model., Work by T.R. was supported by the Deutsche Forschungsgemeinschaft Grant No. Ra 3025/1-1 from the Deutsche Forschungsgemeinschaft. Work by D.V. was supported by National Science Foundation Grant DMR-1954856. Work by I.S. was supported by Grant No. FIS2016-77188-P from the Spanish Ministerio de Economía y Competitividad.

Complementary to bulk synthesis, here we propose a designer lattice with extremely high magnetic frustration and demonstrate the possible realization of a quantum spin liquid state from both experiments and theoretical calculations. In an ultrathin (111) CoCr2O4 slice composed of three triangular and one kagome cation planes, the absence of a spin ordering or freezing transition is demonstrated down to 0.03 K, in the presence of strong antiferromagnetic correlations in the energy scale of 30 K between Co and Cr sublattices, leading to the frustration factor of ∼1000. Persisting spin fluctuations are observed at low temperatures via low-energy muon spin relaxation. Our calculations further demonstrate the emergence of highly degenerate magnetic ground states at the 0 K limit, due to the competition among multiply altered exchange interactions. These results collectively indicate the realization of a proximate quantum spin liquid state on the synthetic lattice.

The modern theory of polarization allows for the determination of the macroscopic end charge of a truncated one-dimensional insulator, modulo the charge quantum e, from a knowledge of bulk properties alone. A more subtle problem is the determination of the corner charge of a two-dimensional insulator, modulo e, from a knowledge of bulk and edge properties alone. While previous works have tended to focus on the quantization of corner charge in the presence of symmetries, here we focus on the case that the only bulk symmetry is inversion, so that the corner charge can take arbitrary values. We develop a Wannier-based formalism that allows the corner charge to be predicted, modulo e, only from calculations on ribbon geometries of two different orientations. We elucidate the dependence of the interior quadrupole and edge dipole contributions upon the gauge used to construct the Wannier functions, finding that while these are individually gauge dependent, their sum is gauge independent. From this we conclude that the edge polarization is not by itself a physical observable and that any Wannier-based method for computing the corner charge requires the use of a common gauge throughout the calculation. We satisfy this constraint using two Wannier construction procedures, one based on projection and another based on a gauge-consistent nested Wannier construction. We validate our theory by demonstrating the correct prediction of corner charge for several tight-binding models. We comment on the relations between our approach and previous ones that have appeared in the literature., Work by S.R. and D.V. was supported by NSF Grant No. DMR-1954856. Work by I.S. was supported by Grant No. FIS2016-77188-P from the Spanish Ministerio de Economía y Competitividad.

Emergent relativistic quasiparticles in Weyl semimetals are the source of exotic electronic properties such as surface Fermi arcs, the anomalous Hall effect and negative magnetoresistance, all observed in real materials. Whereas these phenomena highlight the effect of Weyl fermions on the electronic transport properties, less is known about what collective phenomena they may support. Here, we report a Weyl semimetal, NdAlSi, that offers an example. Using neutron diffraction, we found a long-wavelength helical magnetic order in NdAlSi, the periodicity of which is linked to the nesting vector between two topologically non-trivial Fermi pockets, which we characterize using density functional theory and quantum oscillation measurements. We further show the chiral transverse component of the spin structure is promoted by bond-oriented Dzyaloshinskii-Moriya interactions associated with Weyl exchange processes. Our work provides a rare example of Weyl fermions driving collective magnetism.

Time-reversal broken Weyl semimetals have attracted much attention recently, but certain aspects of their behavior, including the evolution of their Fermi surface topology and anomalous Hall conductivity with Fermi-level position, have remained underexplored. A promising route to obtain such materials may be to start with a nonmagnetic Dirac semimetal and break time-reversal symmetry via magnetic doping or magnetic proximity. Here we explore this scenario in the case of the Dirac semimetal ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ based on first-principles density-functional calculations and subsequent low-energy modeling of ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ in the presence of a Zeeman field applied along the symmetry axis. We clarify how each fourfold degenerate Dirac node splits into four Weyl nodes, two with chirality $\ifmmode\pm\else\textpm\fi{}1$ and two higher-order nodes with chirality $\ifmmode\pm\else\textpm\fi{}2$. Using a minimal $k\ifmmode\cdot\else\textperiodcentered\fi{}p$ model Hamiltonian whose parameters are fit to the first-principles calculations, we detail the evolution of the Fermi surfaces and their Chern numbers as the Fermi energy is scanned across the region of the Weyl nodes at fixed Zeeman field. We also compute the intrinsic anomalous Hall conductivity as a function of the Fermi-level position, finding a characteristic inverted-dome structure. ${\mathrm{Cd}}_{3}{\mathrm{As}}_{2}$ is especially well suited to such a study because of its high mobility, but the qualitative behavior revealed here should be applicable to other Dirac semimetals as well.

Author(s): Neal, SN; Kim, HS; O'Neal, KR; Haglund, AV; Smith, KA; Mandrus, DG; Bechtel, HA; Carr, GL; Haule, K; Vanderbilt, D; Musfeldt, JL | Abstract: We employ synchrotron-based near-field infrared spectroscopy to reveal the vibrational properties of bulk, few-sheet, and single-sheet members of the MPS3 (M=Mn, Fe, Ni) family of materials and compare our findings with complementary lattice dynamics calculations. MnPS3 and the Fe analog are similar in terms of their symmetry crossovers, from C2/m to P3¯1m, as the monolayer is approached. These states differ as to the presence of a C3 rotation around the metal center. On the other hand, NiPS3 does not show a symmetry crossover, and the lack of a Bu symmetry mode near 450 cm-1 suggests that C3 rotational symmetry is already present, even in the bulk material. We discuss these findings in terms of local symmetry and temperature effects as well as the curious relationship between these symmetry transformations and those that take place under pressure.

MoTe_{2} has recently attracted much attention due to the observation of pressure-induced superconductivity, exotic topological phase transitions, and nonlinear quantum effects. However, there has been debate on the intriguing structural phase transitions among various observed phases of MoTe_{2} and their connection to the underlying topological electronic properties. In this work, by means of density-functional theory calculations, we investigate the structural phase transition between the polar T_{d} and nonpolar 1T^{'} phases of MoTe_{2} in reference to a hypothetical high-symmetry T_{0} phase that exhibits higher-order topological features. In the T_{d} phase we obtain a total of 12 Weyl points, which can be created/annihilated, dynamically manipulated, and switched by tuning a polar phonon mode. We also report the existence of a tunable nonlinear Hall effect in T_{d}-MoTe_{2} and propose the use of this effect as a probe for the detection of polarity orientation in polar (semi)metals. By studying the role of dimensionality, we identify a configuration in which a nonlinear surface response current emerges. The potential technological applications of the tunable Weyl phase and the nonlinear Hall effect are discussed.

Here, we present microscopic evidence of the persistence of uniaxial A-type antiferromagnetic order to the surface layers of MnBi_{2}Te_{4} single crystals using magnetic force microscopy. Our results reveal termination-dependent magnetic contrast across both surface step edges and domain walls, which can be screened by thin layers of soft magnetism. The robust surface A-type order is further corroborated by the observation of termination-dependent surface spin-flop transitions, which have been theoretically proposed decades ago. Our results not only provide key ingredients for understanding the electronic properties of the antiferromagnetic topological insulator MnBi_{2}Te_{4}, but also open a new paradigm for exploring intrinsic surface metamagnetic transitions in natural antiferromagnets.

We have carried out neutron diffraction and small-angle neutron scattering measurements on a high-quality single crystal of the cubic lacunar spinel multiferroic, ${\mathrm{GaV}}_{4}{\mathrm{S}}_{8}$, as a function of magnetic field and temperature to determine the magnetic properties for the single electron that is located on the tetrahedrally coordinated ${\mathrm{V}}_{4}$ molecular unit. Our results are in good agreement with the structural transition at 44 K from cubic to rhombohedral symmetry where the system becomes a robust ferroelectric, while long-range magnetic order develops below 13 K in the form of an incommensurate cycloidal magnetic structure, which can transform into a N\'eel-type skyrmion phase in a modest applied magnetic field. Below 5.9(3) K, the crystal enters a ferromagnetic phase, and we find the magnetic order parameter indicates a long-range-ordered ground state with an ordered moment of 0.23(1) ${\ensuremath{\mu}}_{\mathrm{B}}$ per V ion. Both polarized and unpolarized neutron data in the ferroelectric-paramagnetic phase have been measured to determine the magnetic form factor. The data are consistent with a model of the single spin being uniformly distributed across the ${\mathrm{V}}_{4}$ molecular unit, rather than residing on the single apical V ion, in substantial agreement with the results of first-principles theory. In the magnetically ordered state, polarized neutron measurements are important since both the cycloidal and ferromagnetic order parameters are clearly coupled to the ferroelectricity, causing the structural peaks to be temperature and field dependent. For the ferromagnetic ground state, the spins are locked along the [1,1,1] direction by a surprisingly large anisotropy.

Here, we present microscopic evidence of the persistence of uniaxial A-type antiferromagnetic order to the surface layers of MnBi_{2}Te_{4} single crystals using magnetic force microscopy. Our results reveal termination-dependent magnetic contrast across both surface step edges and domain walls, which can be screened by thin layers of soft magnetism. The robust surface A-type order is further corroborated by the observation of termination-dependent surface spin-flop transitions, which have been theoretically proposed decades ago. Our results not only provide key ingredients for understanding the electronic properties of the antiferromagnetic topological insulator MnBi_{2}Te_{4}, but also open a new paradigm for exploring intrinsic surface metamagnetic transitions in natural antiferromagnets.

Nonreciprocal directional dichroism is an unusual light–matter interaction that gives rise to diode-like behavior in low-symmetry materials. The chiral varieties are particularly scarce due to the requirements for strong spin–orbit coupling, broken time-reversal symmetry, and a chiral axis. Here we bring together magneto-optical spectroscopy and first-principles calculations to reveal high-energy, broadband nonreciprocal directional dichroism in Ni3TeO6 with special focus on behavior in the metamagnetic phase above 52 T. In addition to demonstrating this effect in the magnetochiral configuration, we explore the transverse magnetochiral orientation in which applied field and light propagation are orthogonal to the chiral axis and, by so doing, uncover an additional configuration with a unique nonreciprocal response in the visible part of the spectrum. In a significant conceptual advance, we use first-principles methods to analyze how the Ni2+d-to-d on-site excitations develop magneto-electric character and present a microscopic model that unlocks the door to theory-driven discovery of chiral magnets with nonreciprocal properties.

We report a polarized Raman scattering study of the lattice dynamics of $\ensuremath{\beta}\ensuremath{-}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ under hydrostatic pressures up to 7.62 GPa. At ambient pressure, $\ensuremath{\beta}\ensuremath{-}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ exhibits the hyperhoneycomb crystal structure and a magnetically ordered state of spin-orbit entangled ${J}_{\mathrm{eff}}$ = 1/2 moments that are strongly influenced by bond-directional (Kitaev) exchange interactions. At a critical pressure of $\ensuremath{\sim}\phantom{\rule{0.16em}{0ex}}4.1$ GPa, the phonon spectrum changes abruptly, consistent with the reported structural transition into a monoclinic, dimerized phase. A comparison to the phonon spectra obtained from density-functional calculations shows reasonable overall agreement. The calculations also indicate that the high-pressure phase is a nonmagnetic insulator driven by the formation of Ir--Ir dimer bonds. Our results thus indicate a strong sensitivity of the electronic properties of $\ensuremath{\beta}\ensuremath{-}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ to the pressure-induced structural transition.

Many magnetic point-group symmetries induce a topological classification on crystalline insulators, dividing them into those that have a nonzero quantized Chern-Simons magnetoelectric coupling (“axion-odd” or “topological”) and those that do not (“axion-even” or “trivial”). For time-reversal or inversion symmetries, the resulting topological state is usually denoted as a “strong topological insulator” or an “axion insulator,” respectively, but many other symmetries can also protect this “axion Z2” index. Topological states are often insightfully characterized by choosing one crystallographic direction of interest and inspecting the hybrid Wannier (or equivalently, the non-Abelian Wilson-loop) band structure, considered as a function of the two-dimensional Brillouin zone in the orthogonal directions. Here, we systematically classify the axion-quantizing symmetries and explore the implications of such symmetries on the Wannier band structure. Conversely, we clarify the conditions under which the axion Z2 index can be deduced from the Wannier band structure. In particular, we identify cases in which a counting of Dirac touchings between Wannier bands, or a calculation of the Chern number of certain Wannier bands, or both, allows for a direct determination of the axion Z2 index. We also discuss when such symmetries impose a “flow” on the Wannier bands, such that they are always glued to higher and lower bands by degeneracies somewhere in the projected Brillouin zone, and the related question of when the corresponding surfaces can remain gapped, thus exhibiting a half-quantized surface anomalous Hall conductivity. Our formal arguments are confirmed and illustrated in the context of tight-binding models for several paradigmatic axion-odd symmetries, including time reversal, inversion, simple mirror, and glide mirror symmetries., Work by N.V. and D.V. was supported by the Institute for Quantum Matter, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, under Award No. DE-SC0019331. Work by I.S. was supported by Grant No. FIS2016-77188-P from the Ministerio de Ciencia e Innovación (Spain).

The switching polarization of a ferroelectric is determined by the current that flows as the system is switched between two variants. Computation of the switching polarization in crystal systems has been enabled by the modern theory of polarization, where it is expressed in terms of a change in Berry phase from the initial state to the final state. It is straightforward to compute this change of phase modulo $2\ensuremath{\pi}$, thus requiring a branch choice to specify the predicted switching polarization. The measured switching polarization depends on the actual path along which the system is switched, which in general involves nucleation and growth of domains and is therefore quite complex. In this work we present a first-principles approach for predicting the switching polarization that requires only knowledge of the initial and final states based on the empirical observation that for most ferroelectrics, the observed polarization change is the same as that for a path involving minimal evolution of the state. To compute the change along a generic minimal path, we decompose the change of Berry phase into many small contributions, each much less than $2\ensuremath{\pi}$, allowing for a natural resolution of the branch choice. We show that for typical ferroelectrics, including those that would have otherwise required a densely sampled path, this technique allows the switching polarization to be computed without any need for intermediate sampling between oppositely polarized states.

We demonstrate that chiral hinge modes naturally emerge in insulating crystals undergoing a slow cyclic evolution that changes the Chern-Simons axion angle θ by 2π. This happens when the surface (not just the bulk) returns to its initial state at the end of the cycle, in which case it must pass through a metallic state to dispose of the excess quantum of surface anomalous Hall conductivity pumped from the bulk. If two adjacent surfaces become metallic at different points along the cycle, there is an interval in which they are in topologically distinct insulating states, with chiral modes propagating along the connecting hinge. We illustrate these ideas for a tight-binding model consisting of coupled layers of the Haldane model with alternating parameters. The surface topology is determined in a slab geometry using two different markers, surface anomalous Hall conductivity and surface-localized charge pumping (flow of surface-localized Wannier bands), and we find that both correctly predict the appearance of gapless hinge modes in a rod geometry. When viewing the axion pump as a four-dimensional crystal with one synthetic dimension, the hinge modes trace Fermi arcs in the Brillouin zone of the two-dimensional hinge connecting a pair of three-dimensional surfaces of the four-dimensional crystal., Work by T.O. was funded by the Danish Independent Research Foundation Grant No. 6108-00464B. Work by T.R. was supported by the Forschungsstipendium Grant No. RA 3025/1-1 from the Deutsche Forschungsgemeinschaft. Work by D.V. was supported by National Science Foundation Grant No. DMR-1954856. Work by I.S. was supported by Grant No. FIS2016-77188-P from the Ministerio de Ciencia e Innovación (Spain).

We report on the emergent magnetic state of (111)-oriented CoCr2O4 ultrathin films sandwiched between Al2O3 spacer layers in a quantum confined geometry. At the two-dimensional crossover, polarized neutron reflectometry reveals an anomalous enhancement of the total magnetization compared to the bulk value. Synchrotron X-ray magnetic circular dichroism measurements demonstrate the appearance of a long-range ferromagnetic ordering of spins on both Co and Cr sublattices. Brillouin function analyses and ab-initio density functional theory calculations further corroborate that the observed phenomena are due to the strongly altered magnetic frustration invoked by quantum confinement effects, manifested by the onset of a Yafet–Kittel-type ordering as the magnetic ground state in the ultrathin limit, which is unattainable in the bulk.

Significance Heterojunctions between dissimilar materials provide an opportunity to generate emergent properties not present in their individual components. These properties are often linked to interfacial charge transfer, an important mechanism allowing one to access and control novel quantum states. Here, we have grown unit-cell scale superlattices composed of 5 d S r I r O 3 and 3 d L a N i O 3 . We have discovered a massive interfacial charge transfer from Ir to Ni, triggering dramatic electronic and magnetic reconstructions at the interface that suppress strong spin–orbit coupling effects normally present in the iridates. These findings call for careful evaluation and reinterpretation of experiments on spin–orbit-driven physics in thin films and heterostructures based on prototypical 5 d transition metal oxides.

Author(s): Neal, SN; Kim, HS; Smith, KA; Haglund, AV; Mandrus, DG; Bechtel, HA; Carr, GL; Haule, K; Vanderbilt, D; Musfeldt, JL | Abstract: We measured the near-field infrared response of MnPS3 in bulk, few-, and single-layer form and compared our findings with traditional far-field vibrational spectroscopies, a symmetry analysis, and first-principles lattice dynamics calculations. Trends in the Bu mode near 450cm-1 are striking, with the disappearance of this structure in the thinnest sheets. Combined with the amplified response of the activated Ag mode and analysis of the Au+Bu features, we find that symmetry is unexpectedly increased in few- and single-sheet MnPS3 due to a restoration of the threefold axes of rotation. Monoclinicity in this system is therefore a consequence of the long-range stacking pattern and temperature rather than local structure.

First-principles calculations are performed to investigate the effect of epitaxial strain on energetic, structural, electrical, electronic, and optical properties of $1\ifmmode\times\else\texttimes\fi{}1$ AlN/ScN superlattices. This system is predicted to adopt four different strain regions exhibiting different properties, including optimization of various physical responses such as piezoelectricity, electro-optic and elasto-optic coefficients, and elasticity. Varying the strain between these four different regions also allows the creation of an electrical polarization in a nominally paraelectric material, as a result of a softening of the lowest optical mode, and even the control of its magnitude up to a giant value. Furthermore, it results in an electronic band gap that cannot only change its nature (direct vs indirect), but also cover a wide range of the electromagnetic spectrum from the blue, through the violet and near ultraviolet, to the middle ultraviolet. These findings thus point out the potential of assembling two different materials inside the same heterostructure to design multifunctionality and striking phenomena.

The anomalous Hall effect (AHE) is a nonlinear Hall effect appearing in magnetic conductors, boosted by internal magnetism beyond what is expected from the ordinary Hall effect. With the recent discovery of the quantized version of the AHE, the quantum anomalous Hall effect (QAHE), in Cr- or V-doped topological insulator (TI) (Sb,Bi)

The polarization and piezoelectric response of the BiTe$X$ ($X$=Cl, Br, and I) layered tellurohalides are computed from first principles. The results confirm a mixed ionic-covalent character of the bonding, and demonstrate that the internal structure within each triple layer is only weakly affected by the external stress, while the changes in the charge distribution with stress produce a substantial negative piezoelectric response. This suggests a new mechanism for negative piezoelectric response that should remain robust even in ultra-thin film form in this class of materials.