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Co-based honeycomb magnets have been actively studied recently for the potential realization of emergent quantum magnetism therein such as the Kitaev spin liquid. Here we employ density functional and dynamical mean-field theory methods to examine a family of the Kitaev magnet candidates BaCo$_2$($X$O$_4$)$_2$ ($X$ = P, As, Sb), where the compound with $X$ = Sb being not synthesized yet. Our study confirms the formation of Mott insulating phase and the $J_{\rm eff}$ = 1/2 spin moments at Co$^{2+}$ sites despite the presence of a sizable amount of trigonal crystal field in all three compounds. The pnictogen substitution from phosphorus to antimony significantly changes the in-plane lattice parameters and direct overlap integral between the neighboring Co ions, leading to the suppression of the Heisenberg interaction. More interestingly, the marginal antiferromagnetic nearest-neighbor Kitaev term changes sign into a ferromagnetic one and becomes sizable at the $X$ = Sb limit. Our study suggests that the pnictogen substitution can be a viable route to continuously tune magnetic exchange interactions and to promote magnetic frustration for the realization of potential spin liquid phases in BaCo$_2$($X$O$_4$)$_2$., Comment: 8 pages, 4 figures

We employ ab-initio electronic structure calculations to investigate the charge-density waves and periodic lattice distortions in bilayer 2H-NbSe$_2$. We demonstrate that the vertical stacking can give rise to a variety of patterns that may lower the symmetry of the charge-density waves exhibited separately by the two composing 1H-NbSe$_2$ monolayers. The general tendency to a spontaneous symmetry breaking observed in the ground state and the first excited states is shown to originate from a non-negligible inter-layer coupling. Simulated images for scanning tunnelling microscopy (STM) as well as diffraction/scattering patterns show signatures of the different stacking orders. This may not only be useful to reinterpret past experiments on surfaces and thin films, but may also be exploited to devise ad-hoc experiments for the investigation of the stacking order in 2H-NbSe$_2$. We anticipate that our analysis does not only apply to the 2H-NbSe$_2$ bilayer, but is also relevant for thin films and bulk, whose smallest centro-symmetric component is indeed the bilayer. Finally, our results illustrate clearly that the vertical stacking is not only important for 1T structures, as exemplified by the metal-to-insulator transition observed in 1T-TaS$_2$, but seems to be a general feature of metallic layered transition metal dichalcogenides as well., Comment: 15 pages, 9 figures

Using first-principles techniques, we study the structural, magnetic and electronic properties of (111)-oriented (LaMnO$_3$)$_{2n}$$\vert$(SrMnO$_3$)$_{n}$ superlattices of varying thickness ($n=2,4,6$). We find that the properties of the thinnest superlattice ($n=2$) are similar to the celebrated half-metallic ferromagnetic alloy La$_{2/3}$Sr$_{1/3}$MnO$_3$, with quenched Jahn-Teller distortions. At intermediate thickness ($n=4$), the $a^{-}a^{-}a^{-}$ tilting pattern transitions to the $a^{-}a^{-}c^{+}$ tilting pattern, driven by the lattice degrees of freedom in the LaMnO$_3$ region. The emergence of the Jahn-Teller modes and the spatial extent needed for their development play a key role in this structural transition. For the largest thickness considered ($n=6$), we unveil an emergent separation of Jahn-Teller and volume-breathing orders in the ground-state structure with the $a^{-}a^{-}c^{+}$ tilting pattern, whereas it vanishes in the antiferromagnetic configurations. The ground state of all superlattices is half-metallic ferromagnetic, not affected by the underlying series of structural transitions. Overall, these results outline a thickness-induced crossover between the physical properties of bulk La$_{2/3}$Sr$_{1/3}$MnO$_3$ and bulk LaMnO$_3$., Comment: 7 pages excluding references, 8 figures

We present a molecular orbital candidate Ba$_{4}$TaMn$_{3}$O$_{12}$ with a face-sharing octahedra trimer, by comparing it with a related compound Ba$_{4}$NbMn$_{3}$O$_{12}$. The synthesis of the polycrystalline powder is optimized by suppressing the secondary impurity phase via x-ray diffraction. Magnetic susceptibility measurements on the optimized samples reveal a weak magnetic hysteresis with magnetic transitions consistent with heat capacity results. The effective magnetic moments from susceptibility indicate a strongly coupled $S=2$ antiferromagnetic trimer at around room temperature, whereas the estimated magnetic entropy from heat capacity suggests the localized $S=3/2$ timer. These results can be explainable by a partial molecular orbital state, in which three $t_{2g}$ electrons are localized in each Mn ion and one $e_{g}$ electron is delocalized over two-end Mn ions of the trimer based on density functional theory calculations. This unconventional 3$d$ orbital state is comprehended as a consequence of competition between the hybrid interatomic orbitals within the Mn trimer and the local moment formation by on-site Coulomb correlations., Comment: 15 pages, 12 figures, 4 tables

By employing first-principles electronic structure calculations we investigate nickelate superlattices [LaNiO$_3$]$_1$/[LaAlO$_3$]$_1$ and [LaNiO$_3$]$_1$/[SrTiO$_3$]$_1$ with (001) orientation under epitaxial tensile strain. Within density functional theory augmented by mean-field treatement of on-site electronic correlations, the ground states show remarkable dependence on the correlation strength and the strain. In the weakly and intermediately correlated regimes with small epitaxial strain, the charge-disproportionated insulating states with antiferromagneitc order is favored over the other orbital and spin ordered phases. On the other hand, in the strongly correlated regime or under the large tensile strain, ferromagnetic spin states with Jahn-Teller orbital order become most stable. The effect from polar interfaces in LaNiO$_3$]$_1$/[SrTiO$_3$]$_1$ is found to be noticeable in our single-layered geometry. Detailed discussion is presented in comparison with previous experimental and theoretical studies., Comment: 9 pages, 8 figures

We report Chern insulating phases emerging from a single layer of layered chalcogenide CrSiTe$_{3}$, a transition metal trichacogenides (TMTC) material, in the presence of charge doping. Due to strong hybridization with Te $p$ orbitals, the spin-orbit coupling effect opens a finite band gap, leading to a nontrivial topology of the Cr $e_{\mathrm{g}}$ conduction band manifold with higher Chern numbers. Our calculations show that quantum anomalous Hall effects can be realized by adding one electron in a formula unit cell of Cr$_{2}$Si$_{2}$Te$_{6}$, equivalent to electron doping by 2.36$\times$10$^{14}$ cm$^{-2}$ carrier density. Furthermore, the doping-induced anomalous Hall conductivity can be controlled by an external magnetic field via spin-orientation-dependent tuning of the spin-orbit coupling. In addition, we find distinct quantum anomalous Hall phases employing tight-binding model analysis, suggesting that CrSiTe$_{3}$ can be a fascinating new platform to realize Chern insulating systems with higher Chern numbers., Comment: 9 pages, 8 figures, and additional supplementary information

The emergence of scalar Higgs-type amplitude modes in systems where symmetry is spontaneously broken has been a highly successful, paradigmatic description of phase transitions, with implications ranging from high-energy particle physics to low-energy condensed matter systems. Here, we uncover two successive high temperature phase transitions in the pyrochlore magnet Nd$_2$Ru$_2$O$_7$ at $T_{\mathrm{N}} = 147$ K and $T^* = 97$ K, that lead to giant phonon instabilities and culminate in the emergence of a highly coherent excitation. This coherent excitation, distinct from other phonons and from conventional magnetic modes, stabilizes at a low energy of 3 meV. We assign it to a collective Higgs-type amplitude mode, that involves bond energy modulations of the Ru$_4$ tetrahedra. Its striking two-fold symmetry, incompatible with the underlying crystal structure, highlights the possibility of multiple entangled broken symmetries.

Candidate materials for Kitaev spin liquid phase have been intensively studied recently because of their potential applications in fault-tolerant quantum computing. Although most of the studies on Kitaev spin liquid have been done in 4$d$ and 5$d$ based transition metal compounds, recently there has been a growing research interest in Co-based quasi-two-dimensional honeycomb magnets, such as BaCo$_2$(AsO$_4$)$_2$ because of formation of spin-orbit-entangled $J_{\rm eff}$ = 1/2 pseudospin moments at Co$^{2+}$ sites and potential realizations of Kitaev-like magnetism therein. Here, we obtain high-accuracy crystal and electronic structure of BaCo$_2$(AsO$_4$)$_2$ by employing a combined density functional and dynamical mean-field theory calculations, which correctly capture the Mott-insulating nature of the target system. We show that Co$^{2+}$ ions form a high spin configuration, $S=3/2$, with an active $L_{\rm eff}=1$ orbital degree of freedom, in the absence of spin-orbit coupling. The size of trigonal distortion within CoO$_6$ octahedra is found to be not strong enough to completely quench the orbital degree of freedom, so that the presence of spin-orbit coupling can give rise to the formation of spin-orbit-entangled moments and the Kitaev exchange interaction. Our finding supports recent studies on potential Kitaev magnetism in this compound and other Co-based layered honeycomb systems., Comment: 10 pages, 10 figures

$\alpha$-RuCl$_3$ has been extensively studied recently because of potential bond-dependent Kitaev magnetic exchange interactions and the resulting quantum spin liquid phase that can be realized therein. It has been known that the covalency between Ru 4$d$- and Cl $p$-orbitals is crucial to induce large Kitaev interactions in this compound, therefore replacing Cl into heavier halogen elements such as Br or I can be a promising way to promote the Kitaev interaction even further. In a timely manner, there have been reports on synthesis of $\alpha$-RuBr$_3$ and $\alpha$-RuI$_3$, which are expected to host the same spin-orbit-entangled orbitals and Kitaev exchange interactions with $\alpha$-RuCl$_3$. Here in this work we investigate electronic structures of $\alpha$-RuCl$_3$, $\alpha$-RuBr$_3$, and $\alpha$-RuI$_3$ in a comparative fashion, focusing on the cooperation of the spin-orbit coupling and on-site Coulomb repulsions to realize the spin-orbit-entangled pseudospin-1/2 at Ru sites. We further estimate magnetic exchange interactions of all three compounds, showing that $\alpha$-RuBr$_3$ can be promising candidates to realize Kitaev spin liquid phases in solid-state systems., Comment: 4 pages, 4 figures

Heterostructures of mixed-valence manganites are still under intense scrutiny, due to the occurrence of exotic quantum phenomena linked to electronic correlation and interfacial composition. For instance, if two anti-ferromagnetic insulators as LaMnO$_3$ and SrMnO$_3$ are grown in a (001)-oriented superlattice, a half-metallic ferromagnet may form, provided that the thickness is sufficiently small to allow tunneling across interfaces. In this article, we employ electronic structure calculations to show that all the layers of a (111)-oriented LaMnO$_3$|SrMnO$_3$ superlattice retain a half-metallic ferromagnetic character for a much larger thickness than in its (001) counterpart. This behavior is shown to be linked to the charge transfer across the interface, favored by the octahedral connectivity between the layers. This also results in a symmetry-induced quenching of the Jahn-Teller distortions, which are replaced by breathing modes. The latter are coupled to charge and spin oscillations, whose components have a pure e g character. Most interestingly, the magnetization reaches its maximum value inside the LaMnO$_3$ region and not at the interface, which is fundamentally different from what observed for the (001) orientation. The analysis of the inter-atomic exchange coupling shows that the magnetic order arises from the double-exchange mechanism, despite competing interactions inside the SrMnO$_3$ region. Finally, the van Vleck distortions and the spin oscillations are found to be crucially affected by the variation of Hund's exchange and charge doping, which allows us to speculate that our system behaves as a Hund's metal, creating an interesting connection between manganites and nickelates., Comment: 24 pages, 6 figures

The realization of Kitaev's honeycomb magnetic model in real materials has become one of the most pursued topics in condensed matter physics and materials science. If found, it is expected to host exotic quantum phases of matter and offers potential realizations of fault$-$tolerant quantum computations. Over the past years, much effort was made on 4d$-$ or 5d$-$ heavy transition metal compounds because of their intrinsic strong spin$-$orbit coupling. But more recently, there have been growing shreds of evidence that the Kitaev model could also be realized in 3d$-$transition metal systems with much weaker spin$-$orbit coupling. This review intends to serve as a guide to this fast$-$developing field focusing on systems with d$^7$ transition metal occupation. It overviews the current theoretical and experimental progress on realizing the Kitaev model in those systems. We examine the recent experimental observations of candidate materials with Co$^{2+}$ ions: e.g., CoPS$_3$, Na$_3$Co$_2$SbO$_6$, and Na$_2$Co$_2$TeO$_6$, followed by a brief review of theoretical backgrounds. We conclude this article by comparing experimental observations with density functional theory (DFT) calculations. We stress the importance of inter$-t_{2g}$ hopping channels and Hund's coupling in the realization of Kitaev interactions in Co$-$based compounds, which has been overlooked in previous studies. This review suggests future directions in the search for Kitaev physics in 3d cobalt compounds and beyond., Comment: 45 pages, 13 figures, accepted as Topical Review in Journal of Physics: Condensed Matter

High-throughput material screening for the discovery and design of novel functional materials requires automatized analyses of theoretical and experimental data. Here we study the subject of human-free analyses of one-dimensional spectroscopic data, {\it e.g.} in the frequency domain, via employing deep convolution neural network. Specifically, we trained various deep convolution neural network and benchmarked their performance in decomposing one-dimensional noisy data into multiple nonorthogonal peaks in an iterative manner, after which a conventional basin-hopping algorithm was applied to further reduce residual fitting error. Among six different network architectures, a variant of "Squeeze-and-excitation" network (SENet) structure that we first propose in this study shows the best performance. Dependency of training performance with respect to the choice of the loss function is also discussed. We conclude by applying our modified SENet model to experimental photoemission spectra of graphene, MoS$_2$, and WS$_2$ and address its potential applications and limitations., Comment: 17 pages, 8 figures

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)., Comment: 5 pages, 5 figures

An emerging phase of matter among the class of topological materials is nodal line semimetal, possessing symmetry-protected one-dimensional gapless lines at the (or close to) the Fermi level in $k$-space. When the $k$-dispersion of the nodal line is weak, van Hove singularities generated by the almost flat nodal lines may be prone to instabilities introduced by additional perturbations such as spin-orbit coupling or magnetism. Here, we study Cr-based ferromagnetic chalcospinel compound CuCr$_2$Se$_4$ (CCS) via first-principles electronic structure methods and reveal the true origin of its dissipationless anomalous Hall conductivity, which was not well understood previously. We find that CCS hosts nodal lines protected by nonsymmorphic symmetries, located in the vicinity of Fermi level, and that such nodal lines are the origin of the previously observed distinct behavior of the anomalous Hall signature in the presence of electron doping. The splitting of nodal line via spin-orbit coupling produces a large Berry curvature, which leads to a significant response in anomalous Hall conductivity. Upon electron doping via chemical substitution or gating, or rotation of magnetization via external magnetic field, steep change of anomalous Hall behavior occurs, which makes CCS a promising compound for low energy spintronics applications., Comment: 9 pages, 10 figures

We report a polarized Raman scattering study of the lattice dynamics of $\beta$-Li$_2$IrO$_3$ under hydrostatic pressures up to 7.62 GPa. At ambient pressure, $\beta$-Li$_2$IrO$_3$ exhibits the hyperhoneycomb crystal structure and a magnetically ordered state of spin-orbit entangled Jeff = 1/2 moments that is strongly influenced by bond-directional (Kitaev) exchange interactions. At a critical pressure of ~ 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 $\beta$-Li$_2$IrO$_3$ to the pressure-induced structural transition., Comment: 16 pages, 7 figures, 5 tables, Supplemental Material included

Finding new materials with antiferromagnetic (AFM) Kitaev interaction is an urgent issue to broaden and enrich the quantum magnetism research significantly. By carrying out inelastic neutron scattering experiments and subsequent analysis, we conclude that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are new honeycomb cobalt-based AFM Kitaev systems. The spin-orbit excitons at 20-28~meV in both compounds strongly supports the idea that Co$^{2+}$ ions of both compounds have a spin-orbital entangled $J_\rm{eff}=1/2$ state. Furthermore, we found that a generalized Kitaev-Heisenberg Hamiltonian can well describe the spin-wave excitations of both compounds with additional 3rd nearest-neighbor interaction. Our best-fit parameters show large AFM Kitaev terms and off-diagonal symmetric anisotropy terms of a similar magnitude in both compounds. We should stress that our parameters' optimized magnetic structures are consistent with the magnetic structures reported from neutron diffraction studies. Moreover, there is also the magnon-damping effect at the higher energy part of the spin waves, as usually observed in other Kitaev magnets. We demonstrate that Na$_3$Co$_2$SbO$_6$ and Na$_2$Co$_2$TeO$_6$ are the first experimental realization of AFM Kitaev magnets based on the systematic studies of the spin waves and analysis., Comment: 28 pages, 10 figures, Journal of Physics: Condensed Matter

The magnetic excitations in CoPS$_3$, a two-dimensional van der Waals (vdW) antiferromagnet with spin $S=3/2$ on a honeycomb lattice, has been measured using powder inelastic neutron scattering. Clear dispersive spin waves are observed with a large spin gap of ~13 meV. The magnon spectra were fitted using an $XXZ$-type $J_1-J_2-J_3$ Heisenberg Hamiltonian with a single-ion anisotropy assuming no magnetic exchange between the honeycomb layers. The best-fit parameters show ferromagnetic exchange $J_1=-2.08$ meV and $J_2=-0.26$ meV for the nearest and second-nearest neighbors and a sizeable antiferromagnetic exchange $J_3=4.21$ meV for the third-nearest neighbor with the strong easy-axis anisotropy $K=-2.06$ meV. The suitable fitting could only be achieved by the anisotropic $XXZ$-type Hamiltonian, in which the exchange interaction for the out-of-plane component is smaller than that for the in-plane one by a ratio $\alpha=J_z/J_x=0.6$. Moreover, the absence of spin-orbit exciton around 30 meV indicates that Co$^{2+}$ ions in CoPS$_3$ have a $S=3/2$ state rather than a spin-orbital entangled $J_\rm{eff}=1/2$ ground state. Our result directly shows that CoPS$_3$ is an experimental realization of the $XXZ$ model with a honeycomb lattice in 2D vdW magnets., Comment: 17 pages, 5 figures

We have carried out neutron diffraction and small angle neutron scattering measurements on a high quality single crystal of the cubic lacunar spinel multiferroic, GaV$_4$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 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) ${\mu}_\mathrm{B}$ 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 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.

We study the thermodynamic and high-magnetic-field properties of the magnetic insulator Ba$_5$CuIr$_3$O$_{12}$, which shows no magnetic order down to 2 K consistent with a spin liquid ground state. While the temperature dependence of the magnetic susceptibility and the specific heat shows only weak antiferromagnetic correlations, we find that the magnetization does not saturate up to a field of 59 Tesla, leading to an apparent contradiction. We demonstrate that the paradox can be resolved, and all of the experimental data can be consistently described within the framework of random singlet states. We demonstrate a generic procedure to derive the exchange coupling distribution $P(J)$ from the magnetization measurements and use it to show that the experimental data is consistent with the power-law form $P(J)\sim J^{-\alpha}$ with $\alpha \approx 0.6 $. Thus, we reveal that high-magnetic-field measurements can be essential to discern quantum spin liquid candidates from disorder dominated states that do not exhibit long-range order.

In this study, we investigated theoretically the Mott-insulating phase of a deficient spinel chalcogenide GaV$_4$S$_8$, which is known to form a tetrahedral V$_4$S$_4$ cluster unit that results in molecular orbitals (MOs) with a narrow bandwidth in the noninteracting limit. We used a cluster extension of charge self-consistent embedded dynamical mean-field theory to study the impact of strong intra-cluster correlations on the spectral properties as well as the structural degrees of freedom of the system. We found that the strong tetrahedral clustering renders the atomic Mott picture ineffective, and that the resulting MO picture is essential to describe the Mott phase. It was also found that, while the spectral properties can be qualitatively described by the truncation of the Hilbert space down to the lowest-energy MO, a proper description of the structural degrees of freedom requires the inclusion of multi-MO correlations that span a larger energy window. Specifically, we found that the lowest-energy MO description overemphasizes the clustering tendency, while the inclusion of the Hund's coupling between the lower- and higher-energy MOs corrects this tendency, bringing the theoretically predicted crystal structure into good agreement with the experiment., Comment: 5 pages, 5 figures

We report $\textit{ab-initio}$ density functional theory calculation and Raman scattering results to explore the electronic structure of Ba$_5$CuIr$_3$O$_{12}$ single crystals. This insulating iridate, consisting of face-sharing IrO$_6$ octahedra forming quasi-one-dimensional chains, cannot be described by the local $j_{\rm eff}$=1/2 moment picture commonly adopted for discussing electronic and magnetic properties of iridate compounds with IrO$_6$ octahedra. The shorter Ir-Ir distance in the face-sharing geometry, compared to corner- or edge-sharing structures, leads to strong covalency between neighboring Ir. Then this strong covalency results in the formation of molecular orbitals (MO) at each Ir trimers as the low-energy electronic degree of freedom. The theoretically predicted three-peak structure in the joint density of states, a distinct indication of deviation from the $j_{\rm eff}$=1/2 picture, is verified by observing the three-peak structure in the electronic excitation spectrum by Raman scattering., Comment: 5 pages, 5 figures, with a Supplementary Information

Transition metal phosphorous trichalcogenides, $M{\rm P}X_3$ ($M$ and $X$ being transition metal and chalcogen elements respectively), have been the focus of substantial interest recently because of their possible magnetism in the two-dimensional limit. Here we investigate material properties of the compounds with $M$ = Mn and Ni employing $\textit{ab-initio}$ density functional and dynamical mean-field calculations, especially their electronic behavior under external pressure in the paramagnetic phase. Mott metal-insulator transitions (MIT) are found to be a common feature for both compounds, but their lattice structures show drastically different behaviors depending on the relevant orbital degrees of freedom, i.e. $t_{\rm 2g}$ or $e_{g}$. MnPS$_3$ undergoes an isosymmetric structural transition by forming Mn-Mn dimers due to the strong direct overlap between the neighboring $t_{\rm 2g}$ orbitals, accompanied by a significant volume collapse and a spin-state transition. In contrast, NiPS$_3$ and NiPSe$_3$, with their active $e_g$ orbital degrees of freedom, do not show a structural change at the MIT pressure or deep in the metallic phase. Hence NiPS$_3$ and NiPSe$_3$ become rare examples of materials hosting electronic bandwidth-controlled Mott MITs, thus showing promise for ultrafast resistivity switching behavior., Comment: 5 pages, 4 figures

Recent developments in topological semimetals open a way to realize relativistic dispersions in condensed matter systems. One recently studied type of topological feature is the "triple nodal point" where three bands become degenerate. In contrast to Weyl and Dirac nodes, triple nodal points, which are protected by a rotational symmetry, have nodal lines attached, so that a characterization in terms of a chirality is not possible. Previous studies of triple nodal points considered nonmagnetic systems, although an artificial Zeeman splitting was used to probe the topological nature. Here instead we treat a ferromagnetic material, half-metallic GdN, where the splitting of the triple nodal points comes from the spin-orbit coupling. The size of the splitting ranges from 15 to 150 meV depending on the magnetization orientation, enabling a transition between a Weyl-point phase and a "nearly triple nodal point" phase that exhibits very similar surface spectra and transport properties compared to a true triple-node system. The rich topological surface states, manipulable via the orientation of the magnetization, make half-metallic GdN a promising platform for future investigations and applications.

We report a comprehensive study on the surface structural and electronic properties of TaTe2 at room temperature. The surface structure was investigated using both low energy electron diffraction intensity versus voltage and density functional theory calculations. The relaxed structures obtained from the two methods are in good agreement, which is very similar to the bulk, maintaining double zigzag trimer chains. The calculated density of states indicates that such structure originates from the trimer bonding states of the Ta dxz and dxy orbitals. This work will further provide new insights towards the understanding of the charge density wave phase transition in TaTe2 at low temperature.

Coexistence of topological elements in a topological metal/semimetal (TM) has gradually attracted attentions. However, the non-topological factors always mess up the Fermi surface and cover interesting topological properties. Here, we find that Ba3Si4 is a "clean" TM in which coexists nodal-chain network, intersecting nodal rings (INRs) and triple points, in the absence of spin-orbit coupling (SOC). Moreover, the nodal rings in the topological phase exhibit diverse types: from type-I, type-II to type-III rings according to band dispersions. All the topological elements are generated by crossings of three energy bands, and thus they are correlated rather than mutual independence. When some structural symmetries are eliminated by an external strain, the topological phase evolves into another phase including Hopf link, one-dimensional nodal chain and new INRs.

The unique properties of topological semimetals have strongly driven efforts to seek for new topological phases and related materials. Here, we identify a critical condition for the existence of linked nodal rings (LNRs) in symmorphic crystals, and propose that three types of LNRs, named as alpha-, beta- and gamma-type, can be obtained by stacking semiconducting layers. Several honeycomb structures are suggested to be topological LNR semimetals, including layered and "hidden" layered structures. Transitions between the three types of LNRs can be driven by external strains. Interesting surface states other than drumhead states are found in these topological materials.

The topological Haldane model (THM) on a honeycomb lattice is a prototype of systems hosting topological phases of matter without external fields. It is the simplest model exhibiting the quantum Hall effect without Landau levels, which motivated theoretical and experimental explorations of topological insulators and superconductors. Despite its simplicity, its realization in condensed matter systems has been elusive due to a seemingly difficult condition of spinless fermions with sublattice-dependent magnetic flux terms. While there have been theoretical proposals including elaborate atomic-scale engineering, identifying candidate THM materials has not been successful, and the first experimental realization was recently made in ultracold atoms. Here we suggest that a series of Fe-based honeycomb ferromagnetic insulators, AFe2(PO4)2 (A=Ba,Cs,K,La) possess Chern bands described by the THM. How to detect the quantum anomalous Hall effect is also discussed., Comment: 5 pages, 3 figures, and 1 table

There have been tremendous experimental and theoretical efforts toward discovery of quantum spin liquid phase in honeycomb-based-lattice materials with strong spin-orbit coupling. Here the bond-dependent Kitaev interaction between local moments provides strong magnetic frustration and if it is the only interaction present in the system, it will lead to an exactly solvable quantum spin liquid ground state. In all of these materials, however, the ground state is in a magnetically ordered phase due to additional interactions between local moments. Recently, it has been reported that the magnetic order in hyperhoneycomb material, $\beta$-Li$_2$IrO$_3$, is suppressed upon applying hydrostatic pressure and the resulting state becomes a quantum paramagnet or possibly a quantum spin liquid. Using ab-initio computations and strong coupling expansion, we investigate the lattice structure and resulting local moment model in pressurized $\beta$-Li$_2$IrO$_3$. Remarkably, the dominant interaction under high pressure is not the Kitaev interaction nor further neighbor interactions, but a different kind of bond-dependent interaction. This leads to strong magnetic frustration and may provide a platform for discovery of a new kind of quantum spin liquid ground state., Comment: 7 pages, 4 figures, and 2 tables

The spin-orbit Mott insulator Sr3Ir2O7 provides a fascinating playground to explore insulator-metal transition driven by intertwined charge, spin, and lattice degrees of freedom. Here, we report high pressure electric resistance and resonant inelastic x ray scattering measurements on single crystal Sr3Ir2O7 up to 63 65 GPa at 300 K. The material becomes a confined metal at 59.5 GPa, showing metallicity in the ab plane but an insulating behavior along the c axis. Such an unusual phenomenon resembles the strange metal phase in cuprate superconductors. Since there is no sign of the collapse of spin orbit or Coulomb interactions in x-ray measurements, this novel insulator metal transition is potentially driven by a first-order structural change at nearby pressures. Our discovery points to a new approach for synthesizing functional materials., Comment: 4-page 3-figure

We study possible edge states in single layers of honeycomb materials such as $\alpha$-RuCl$_3$ and A$_2$IrO$_3$ (A=Li, Na) with strong spin-orbit coupling (SOC). These two dimensional systems exhibit linearly dispersing one-dimensional (1D) edge states when their 1D boundary forms a zig-zag shape. Using an effective tight-binding model based on first principles band structure calculations including Hubbard U and SOC, we find degenerate edge states at the zone center and zone boundary. The roles of chiral symmetry and time-reversal symmetry are presented. The implications to experimental signatures and the effects of disorder are also discussed., Comment: 5 pages, 2 tables, 4 figures

$\alpha$-RuCl$_3$ has been hinted as a spin-orbital-assisted Mott insulator in proximity to a Kitaev spin liquid state. Here we present ARPES measurements on single crystal $\alpha$-RuCl$_3$ in both the pristine and electron-doped states, and combine them with LDA+SOC+U calculations performed for the several low-energy competing magnetically ordered states as well as the paramagnetic state. A large Mott gap is found in the measured band structure of the pristine compound that persists to more than 20 times beyond the magnetic ordering temperature, though the paramagnetic calculation shows almost no gap. Upon electron doping, spectral weight is transferred into the gap but the new states still maintain a sizable gap from the Fermi edge. These findings are most consistent with a Mott insulator with a somewhat exotic evolution out of the Mott state with both temperature and doping, likely related to unusually strong spin fluctuations., Comment: 5 pages, 6 figures in main text. 3 pages, 2 figures in supplementary information

Numerous efforts have been devoted to reveal exotic semimetallic phases with topologically non-trivial bulk and/or surface states in materials with strong spin-orbit coupling. In particular, semimetals with nodal line Fermi surface (FS) exhibit novel properties, and searching for candidate materials becomes an interesting research direction. Here we provide a generic condition for a four-fold degenerate nodal line FS in non-symmorphic crystals with inversion and time-reversal symmetry (TRS). When there are two glide planes or screw axes perpendicular to each other, a pair of Bloch bands related by non-symmorphic symmetry become degenerate on a Brillouin Zone (BZ) boundary. There are two pairs of such bands, and they disperse in a way that the partners of two pairs are exchanged on other BZ boundaries. This enforces a nodal line FS on a BZ boundary plane protected by non-symmorphic symmetries. When TRS is broken, four-fold degenerate Dirac points or Weyl ring FS could occur depending on a direction of the magnetic field. On a certain surface double helical surface states exist, which become double Ferm arcs as TRS is broken., Comment: 6 pages, 4 figures

$\alpha$-RuCl$_3$ has been proposed recently as an excellent playground for exploring Kitaev physics on a two-dimensional (2D) honeycomb lattice. However, structural clarification of the compound has not been completed, which is crucial in understanding the physics of this system. Here, using {\it ab-initio} electronic structure calculations, we study a full three dimensional (3D) structure of $\alpha$-RuCl$_3$ including the effects of spin-orbit coupling (SOC) and electronic correlations. Three major results are as follows; i) SOC suppresses dimerization of Ru atoms, which exists in other Ru compounds such as isostructural Li$_2$RuO$_3$, and making the honeycomb closer to an ideal one. ii) The nearest-neighbor Kitaev exchange interaction between the $j_{\rm eff}$=1/2 pseudospin depends strongly on the Ru-Ru distance and the Cl position, originating from the nature of the edge-sharing geometry. iii) The optimized 3D structure without electronic correlations has $P{\bar 3}1m$ space group symmetry independent of SOC, but including electronic correlation changes the optimized 3D structure to either $C2/m$ or $Cmc2_1$ within 0.1 meV per formula unit (f.u.) energy difference. The reported $P3_112$ structure is also close in energy. The interlayer spin exchange coupling is a few percent of in-plane spin exchange terms, confirming $\alpha$-RuCl$_3$ is close to a 2D system. We further suggest how to increase the Kitaev term via tensile strain, which sheds new light in realizing Kitaev spin liquid phase in this system., Comment: 10 pages, 10 figures, and 4 tables

Ordered phases such as charge- and spin-density wave state accompany either full or partial gapping of Fermi surface (FS) leading a metal-insulator or metal-metal transition (MMT). However, there are examples of MMT without any signatures of symmetry breaking. One example is Na$_2$Ti$_2$Sb$_2$O, where a partial gapping of FS is observed but a density wave ordering has not been found. Here we propose a microscopic mechanism of such a MMT which occurs due to a momentum dependent spin-orbit coupled molecular orbital polarization. Since a molecular $d$ orbital polarization is present due to a small spin-orbit coupling of Ti, there is no spontaneous symmetry breaking involved. However, a sharp increase of polarization happens above a critical electron interaction which gaps out the $d$ orbtial FS and reduces the density of states significantly, while the rest of FS associated with Sb $p$ orbtials is almost intact across MMT. Experimental implications to test our proposal and applications to other systems are also discussed., Comment: 5 pages, 3 figures

Frustrated transition metal compounds in which spin-orbit coupling (SOC) and electron correlation work together have attracted much attention recently. In the case of 5$d$ transition metals, where SOC is large, $j_\text{eff}=1/2$ bands near the Fermi level are thought to encompass the essential physics of the material, potentially leading to a concrete realization of exotic magnetic phases such as the Kitaev spin liquid. Here we derive a spin model on a triangular lattice based on $j_\text{eff} = 1/2$ pseudospins that interact via antiferromagnetic Heisenberg ($J$) and Kitaev ($K$) exchanges, and crucially, an anisotropic $(\Gamma)$ exchange. Our classical analysis of the spin model reveals that, in addition to small regions of 120$^\circ$, $\mathbb{Z}_2$ / dual-$\mathbb{Z}_2$ vortex crystal and nematic phases, the stripy and ferromagnetic phases dominate the $J$-$K$-$\Gamma$ phase diagram. We apply our model to the 5$d$ transition metal compound, Ba$_3$IrTi$_2$O$_9$, in which the Ir$^{4+}$ ions form layered two-dimensional triangular lattices. We compute the band structure and nearest-neighbor hopping parameters using ab-initio calculations. By combining our ab-initio and classical analyses, we predict that Ba$_3$IrTi$_2$O$_9$ has a stripy ordered magnetic ground state., Comment: 8 pages, 5 figures

Mott insulators with strong spin-orbit coupling have been proposed to host unconventional magnetic states, including the Kitaev quantum spin liquid. The 4$d$ system $\alpha$-RuCl$_3$ has recently come into view as a candidate Kitaev system, with evidence for unusual spin excitations in magnetic scattering experiments. We apply a combination of optical spectroscopy and Raman scattering to study the electronic structure of this material. Our measurements reveal a series of orbital excitations involving localized total angular momentum states of the Ru ion, implying that strong spin-orbit coupling and electron-electron interactions coexist in this material. Analysis of these features allows us to estimate the spin-orbit coupling strength, as well as other parameters describing the local electronic structure, revealing a well-defined hierarchy of energy scales within the Ru $d$ states. By comparing our experimental results with density functional theory calculations, we also clarify the overall features of the optical response. Our results demonstrate that $\alpha$-RuCl$_3$ is an ideal material system to study spin-orbit coupled magnetism on the honeycomb lattice., Comment: 7 pages, 4 figures, v2: revised figures and discussion, matches published version

The recently discovered three-dimensional hyperhoneycomb iridate, $\beta$-Li$_2$IrO$_3$, has raised hopes for the realization of dominant Kitaev interaction between spin-orbit entangled local moments due to its near-ideal lattice structure. If true, this material may lie close to the sought-after quantum spin liquid phase in three dimensions. Utilizing ab-initio electronic structure calculations, we first show that the spin-orbit entangled basis, $j_{\rm eff}$=1/2, correctly captures the low energy electronic structure. The effective spin model derived in the strong coupling limit supplemented by the ab-initio results is shown to be dominated by the Kitaev interaction. We demonstrated that the possible range of parameters is consistent with a non-coplanar spiral magnetic order found in a recent experiment. All of these analyses suggest that $\beta$-Li$_2$IrO$_3$ may be the closest among known materials to the Kitaev spin liquid regime., Comment: 9 pages, 6 figures, 2 tables

Intensive studies of the interplay between spin-orbit coupling (SOC) and electronic correlations in transition metal compounds have recently been undertaken. In particular, $j_{\rm eff}$ = 1/2 bands on a honeycomb lattice provide a pathway to realize Kitaev's exactly solvable spin model. However, since current wisdom requires strong atomic SOC to make $j_{\rm eff}=1/2$ bands, studies have been limited to iridium oxides. Contrary to this expectation, we demonstrate how Kitaev interactions arise in 4$d$-orbital honeycomb $\alpha$-RuCl$_3$, despite having significantly weaker SOC than the iridium oxides, via assistance from electron correlations. A strong coupling spin model for these correlation-assisted $j_{\rm eff}$ = 1/2 bands is derived, in which large antiferromagnetic Kitaev interactions emerge along with ferromagnetic Heisenberg interactions. Our analyses suggest that the ground state is a zigzag-ordered phase lying close to the antiferromagnetic Kitaev spin liquid. Experimental implications for angle resolved photoemission spectroscopy, neutron scattering, and optical conductivities are discussed., Comment: 8 pages, 5 figures, Accepted in Phys. Rev. B Rapid communications

There have been increasing efforts in realizing topological metallic phases with nontrivial surface states. It was suggested that orthorhombic perovskite iridates are classified as a topological crystalline metal (TCM) with flat surface states protected by lattice symmetries. Here we perform first-principles electronic structure calculations for epitaxially stabilized orthorhombic perovskite iridates. Remarkably, two different types of topological surface states are found depending on surface directions. On side surfaces, flat surface states protected by lattice symmetries emerge, manifesting the topological crystalline character. On the top surface, on the other hand, an unexpected Dirac cone appears, indicating surface states protected by a time-reversal symmetry, which is confirmed by the presence of a nontrivial topological $\mathbb{Z}_2$ index. These results suggest that the orthorhombic iridates are unique systems exhibiting both lattice- and global-symmetry-protected topological phases and surface states. Transitions to weak and strong topological insulators and implications of surface states in light of angle resolved photoemission spectroscopy are also discussed., Comment: 7 pages, 7 figures