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Description, We observe magnetotransport coupled to noncoplanar spin ordering/fluctuation in a triangular-lattice magnetic semiconductor., While anomalous Hall effect (AHE) has been extensively studied in the past, efforts for realizing large Hall response have been mainly limited within intrinsic mechanism. Lately, however, a theory of extrinsic mechanism has predicted that magnetic scattering by spin cluster can induce large AHE even above magnetic ordering temperature, particularly in magnetic semiconductors with low carrier density, strong exchange coupling, and finite spin chirality. Here, we find out a new magnetic semiconductor EuAs, where Eu2+ ions with large magnetic moments form distorted triangular lattice. In addition to colossal magnetoresistance, EuAs exhibits large AHE with an anomalous Hall angle of 0.13 at temperatures far above antiferromagnetic ordering. As also demonstrated by model calculations, observed AHE can be explained by the spin cluster scattering in a hopping regime. Our findings shed light on magnetic semiconductors hosting topological spin textures, developing a field targeting diluted carriers strongly coupled to noncoplanar spin structures.

The quest for nonmagnetic Weyl semimetals with high tunability of phase has remained a demanding challenge. As the symmetry breaking control parameter, the ferroelectric order can be steered to turn on/off the Weyl semimetals phase, adjust the band structures around the Fermi level, and enlarge/shrink the momentum separation of Weyl nodes which generate the Berry curvature as the emergent magnetic field. Here, we report the realization of a ferroelectric nonmagnetic Weyl semimetal based on indium doped Pb1 xSnxTe alloy where the underlying inversion symmetry as well as mirror symmetry is broken with the strength of ferroelectricity adjustable via tuning indium doping level and Sn/Pb ratio. The transverse thermoelectric effect, i.e., Nernst effect both for out of plane and in plane magnetic field geometry, is exploited as a Berry curvature sensitive experimental probe to manifest the generation of Berry curvature via the redistribution of Weyl nodes under magnetic fields. The results demonstrate a clean non-magnetic Weyl semimetal coupled with highly tunable ferroelectric order, providing an ideal platform for manipulating the Weyl fermions in nonmagnetic system., 20 pages, 4 figures

Transition metals, Fe, Co and Ni, are the canonical systems for studying the effect of external perturbations on ferromagnetism. Among these, Ni stands out as it undergoes no structural phase transition under pressure. Here we have investigated the long-debated issue of pressure-induced magnetisation drop in Ni from first-principles. Our calculations confirm an abrupt quenching of magnetisation at high pressures, not associated with any structural phase transition. We find that the pressure substantially enhances the crystal field splitting of Ni-$3d$ orbitals, driving the system towards a new metallic phase violating the Stoner Criterion for ferromagnetic ordering. Analysing the charge populations in each spin channel, we show that the next nearest neighbour interactions play a crucial role in quenching ferromagnetic ordering in Ni and materials alike., 5 pages, 5 figures

Topologically nontrivial materials host protected edge states associated with the bulk band inversion through the bulk-edge correspondence. Manipulating such edge states is highly desired for developing new functions and devices practically using their dissipation-less nature and spin-momentum locking. Here we introduce a transition-metal dichalcogenide VTe$_2$, that hosts a charge density wave (CDW) coupled with the band inversion involving V3$d$ and Te5$p$ orbitals. Spin- and angle-resolved photoemission spectroscopy with first-principles calculations reveal the huge anisotropic modification of the bulk electronic structure by the CDW formation, accompanying the selective disappearance of Dirac-type spin-polarized topological surface states that exist in the normal state. Thorough three dimensional investigation of bulk states indicates that the corresponding band inversion at the Brillouin zone boundary dissolves upon CDW formation, by transforming into anomalous flat bands. Our finding provides a new insight to the topological manipulation of matters by utilizing CDWs' flexible characters to external stimuli., Comment: 46 pages, 6 main figures, 12 supplementary figures

Charge density wave (CDW) is a startling quantum phenomenon, distorting a metallic lattice into an insulating state with a periodically modulated charge distribution. Astonishingly, such modulations appear in various patterns even within the same family of materials. Moreover, this phenomenon features a puzzling diversity in its dimensional evolution. Here, we propose a general framework, unifying distinct trends of CDW ordering in an isoelectronic group of materials, 2H-MX2 (M = Nb, Ta and X = S, Se). We show that while NbSe2 exhibits a strongly enhanced CDW order in two dimensions, TaSe2 and TaS2 behave oppositely, with CDW being absent in NbS2 entirely. Such a disparity is demonstrated to arise from a competition of ionic charge transfer, electron-phonon coupling, and electron correlation. Despite its simplicity, our approach can, in principle, explain dimensional dependence of CDW in any material, thereby shedding new light on this intriguing quantum phenomenon and its underlying mechanisms., The dimensional dependence of charge density wave (CDW) in two-dimensional dichalcogenides remains puzzled. Here, Lin et al. study trends of CDW ordering in an isoelectronic group of materials 2H-MX2 and provide a unified understanding involving several microscopic factors.

GeTe is a chemically simple IV-VI semiconductor which bears a rich plethora of different physical properties induced by doping and external stimuli. These include, among others, ferromagnetism, ferroelectricity, phase-change memory functionality, and comparably large thermoelectric figure of merits. Here we report a superconductor - semiconductor - superconductor transition controlled by finely-tuned In doping. Our results moreover show the existence of a critical doping concentration around $x = 0.12$ in Ge$_{1-x}$In$_{x}$Te, where various properties take either an extremum or change their characters: The structure changes from polarly-rhombohedral to cubic, the resistivity sharply increases by orders of magnitude, the type of charge carriers changes from holes to electrons, and the density of states diminishes at the dawn of an emerging superconducting phase. By core-level photoemission spectroscopy we find indications of a change in the In-valence state from In$^{3+}$ to In$^{1+}$ with increasing $x$, suggesting that this system is a new promising playground to probe valence fluctuations and their possible impact on superconductivity., Comment: Main text (4 Figures) + Supplement(9 Figures)

A bulk superconductor possessing a topological surface state at the Fermi level is a promising system to realise long-sought topological superconductivity. Although several candidate materials have been proposed, experimental demonstrations concurrently exploring spin textures and superconductivity at the surface have remained elusive. Here we perform spectroscopic-imaging scanning tunnelling microscopy on the centrosymmetric superconductor β-PdBi2 that hosts a topological surface state. By combining first-principles electronic-structure calculations and quasiparticle interference experiments, we determine the spin textures at the surface, and show not only the topological surface state but also all other surface bands exhibit spin polarisations parallel to the surface. We find that the superconducting gap fully opens in all the spin-polarised surface states. This behaviour is consistent with a possible spin-triplet order parameter expected for such in-plane spin textures, but the observed superconducting gap amplitude is comparable to that of the bulk, suggesting that the spin-singlet component is predominant in β-PdBi2., Although several materials have been proposed as topological superconductors, spin textures and superconductivity at the surface remain elusive. Here, Iwaya et al. determine the spin textures at the surface of a superconductor β-PdBi2 and find the superconducting gap opening in all spin-polarised surface states.

We found that a high mobility semimetal 1T'-MoTe2 shows a significant pressure-dependent change in the cryogenic thermopower in the vicinity of the critical pressure, where the polar structural transition disappears. With the application of a high pressure of 0.75 GPa, while the resistivity becomes as low as 10 {\mu}{\Omega}cm, thermopower reached the maximum value of 60 {\mu}VK-1 at 25 K, leading to a giant thermoelectric power factor of 300 {\mu}WK-2cm-1. Based on semiquantitative analyses, the origin of this behavior is discussed in terms of inelastic electron-phonon scattering enhanced by the softening of zone center phonon modes associated with the polar structural instability., Comment: 13 pages, 4 figures Physical review B (accepted)

Advanced electronic materials 5(5), 1800860 - (2019). doi:10.1002/aelm.201800860, 2D electron gases (2DEGs) in oxides show great potential for the discoveryof new physical phenomena and at the same time hold promise for electronicapplications. In this work, angle-resolved photoemission is used to determinethe electronic structure of a 2DEG stabilized in the (111)-oriented surface ofthe strong spin–orbit coupling material KTaO3. The measurements revealmultiple sub-bands that emerge as a consequence of quantum confinementand form a sixfold symmetric Fermi surface. This electronic structure is wellreproduced by self-consistent tight-binding supercell calculations. Based onthese calculations, the spin and orbital texture of the 2DEG is determined.It is found that the 2DEG Fermi surface is derived from bulk J = 3/2 statesand exhibits an unconventional anisotropic Rashba-like lifting of the spindegeneracy.Spin-momentum locking holds only for high-symmetry directionsand a strong out-of-plane spin component renders the spin texture threefoldsymmetric. It is found that the average spin-splitting on the Fermi surfaceis an order of magnitude larger than in SrTiO3, which should translateinto an enhancement in the spin–orbitronic response of (111)-KTaO3 2DEGbaseddevices., Published by Wiley, Chichester

Magnetic semiconductors are a vital component in the understanding of quantum transport phenomena. To explore such delicate, yet fundamentally important, effects, it is crucial to maintain a high carrier mobility in the presence of magnetic moments. In practice, however, magnetization often diminishes the carrier mobility. Here, it is shown that EuTiO3 is a rare example of a magnetic semiconductor that can be desirably grown using the molecular beam epitaxy to possess a high carrier mobility exceeding 3000 cm2 V-1 s-1 at 2 K, while intrinsically hosting a large magnetization value, 7 μB per formula unit. This is demonstrated by measuring the Shubnikov-de Haas (SdH) oscillations in the ferromagnetic state of EuTiO3 films with various carrier densities. Using first-principles calculations, it is shown that the observed SdH oscillations originate genuinely from Ti 3d-t2g states which are fully spin-polarized due to their energetical proximity to the in-gap Eu 4f bands. Such an exchange coupling is further shown to have a profound effect on the effective mass and fermiology of the Ti 3d-t2g electrons, manifested by a directional anisotropy in the SdH oscillations. These findings suggest that EuTiO3 film is an ideal magnetic semiconductor, offering a fertile field to explore quantum phenomena suitable for spintronic applications.

We develop the realistic minimal electronic model for recently discovered BiS$_2$ superconductors including the spin-orbit coupling based on a first-principles band structure calculations. Due to strong spin-orbit coupling, characteristic for the Bi-based systems, the tight-binding low-energy model necessarily includes $p_x$, $p_y$, and $p_z$ orbitals. We analyze a potential Cooper-pairing instability from purely repulsive interaction for the moderate electronic correlations using the so-called leading angular harmonics approximation (LAHA). For small and intermediate doping concentrations we find the dominant instabilities to be $d_{x^2-y^2}$-wave, and $s_{\pm}$-wave symmetries, respectively. At the same time, in the absence of the sizable spin fluctuations the intra and interband Coulomb repulsion are of the same strength, which yields the strongly anisotropic behaviour of the superconducting gaps on the Fermi surface in agreement with recent ARPES findings. In addition, we find that the Fermi surface topology for BiS$_2$ layered systems at large electron doping can resembles the doped iron-based pnictide superconductors with electron and hole Fermi surfaces with sufficient nesting between them. This could provide further boost to increase $T_c$ in these systems., Comment: 10 pages, 3 figures

We study the low-energy surface electronic structure of the transition-metal dichalcogenide superconductor PdTe$_2$ by spin- and angle-resolved photoemission, scanning tunneling microscopy, and density-functional theory-based supercell calculations. Comparing PdTe$_2$ with its sister compound PtSe$_2$, we demonstrate how enhanced inter-layer hopping in the Te-based material drives a band inversion within the anti-bonding p-orbital manifold well above the Fermi level. We show how this mediates spin-polarised topological surface states which form rich multi-valley Fermi surfaces with complex spin textures. Scanning tunneling spectroscopy reveals type-II superconductivity at the surface, and moreover shows no evidence for an unconventional component of its superconducting order parameter, despite the presence of topological surface states., 6 pages, 3 figures

Tunable bandgaps, extraordinarily large exciton-binding energies, strong light-matter coupling and a locking of the electron spin with layer and valley pseudospins have established transition-metal dichalcogenides (TMDs) as a unique class of two-dimensional (2D) semiconductors with wide-ranging practical applications. Using angle-resolved photoemission (ARPES), we show here that doping electrons at the surface of the prototypical strong spin-orbit TMD WSe2, akin to applying a gate voltage in a transistor-type device, induces a counterintuitive lowering of the surface chemical potential concomitant with the formation of a multivalley 2D electron gas (2DEG). These measurements provide a direct spectroscopic signature of negative electronic compressibility (NEC), a result of electron-electron interactions, which we find persists to carrier densities approximately three orders of magnitude higher than in typical semiconductor 2DEGs that exhibit this effect. An accompanying tunable spin splitting of the valence bands further reveals a complex interplay between single-particle band-structure evolution and many-body interactions in electrostatically doped TMDs. Understanding and exploiting this will open up new opportunities for advanced electronic and quantum-logic devices.

Ferroelectric polarization and metallic conduction are two seemingly irreconcilable properties that cannot normally coexist in a single system, as the latter tends to screen the former. Polar metals, however, defy this rule and have thus attracted considerable attention as a new class of ferroelectrics exhibiting novel properties. Here, we fabricate a new polar metal film based on the typical ferroelectric material BaTiO3by combining chemical doping and epitaxial strain induced by a substrate. The temperature dependences of the c-axis lattice constant and the second harmonic generation intensity of La-doped BaTiO3films indicate the existence of polar transitions. In addition, through La doping, films become metallic at the polar phase, and metallicity enhancement at the polar state occurs in low-La-doped films. This intriguing behaviour is effectively explained by our first-principles calculations. Our demonstration suggests that the carrier doping to ferroelectric material with epitaxial strain serves as a new way to explore polar metals.

The relation between the polar structural instability and superconductivity in a Weyl semimetal candidate MoTe2 has been clarified by finely controlled physical and chemical pressure. The physical pressure as well as the chemical pressure, i.e., the Se substitution for Te, enhances the superconducting transition temperature Tc at around the critical pressure where the polar structure transition disappears. From the heat capacity and thermopower measurements, we ascribe the significant enhancement of Tc at the critical pressure to a subtle modification of the phonon dispersion or the semimetallic band structure upon the polar-to-nonpolar transition. On the other hand, the physical pressure, which strongly reduces the interlayer distance, is more effective on the suppression of the polar structural transition and the enhancement of Tc as compared with the chemical pressure, which emphasizes the importance of the interlayer coupling on the structural and superconducting instability in MoTe2., 5 pages, 4 figures

Transition-metal dichalcogenides (TMDs) are renowned for their rich and varied properties. They range from metals and superconductors to strongly spin-orbit-coupled semiconductors and charge-density-wave systems, with their single-layer variants one of the most prominent current examples of two-dimensional materials beyond graphene. Their varied ground states largely depend on the transition metal d-electron-derived electronic states, on which the vast majority of attention has been concentrated to date. Here, we focus on the chalcogen-derived states. From density-functional theory calculations together with spin- and angle- resolved photoemission, we find that these generically host type-II three-dimensional bulk Dirac fermions as well as ladders of topological surface states and surface resonances. We demonstrate how these naturally arise within a single p-orbital manifold as a general consequence of a trigonal crystal field, and as such can be expected across a large number of compounds. Already, we demonstrate their existence in six separate TMDs, opening routes to tune, and ultimately exploit, their topological physics., 10 pages, 4 figures

Unusual enhancement of cryogenic thermopower manifests itself around the critical point of polar order in a metal., Ferroelectrics with spontaneous electric polarization play an essential role in today’s device engineering, such as capacitors and memories. Their physical properties are further enriched by suppressing the long-range polar order, as exemplified by quantum paraelectrics with giant piezoelectric and dielectric responses at low temperatures. Likewise in metals, a polar lattice distortion has been theoretically predicted to give rise to various unusual physical properties. However, to date, a “ferroelectric”-like transition in metals has seldom been controlled, and hence, its possible impacts on transport phenomena remain unexplored. We report the discovery of anomalous enhancement of thermopower near the critical region between the polar and nonpolar metallic phases in 1T′-Mo1−xNbxTe2 with a chemically tunable polar transition. It is unveiled from the first-principles calculations and magnetotransport measurements that charge transport with a strongly energy-dependent scattering rate critically evolves toward the boundary to the nonpolar phase, resulting in large cryogenic thermopower. Such a significant influence of the structural instability on transport phenomena might arise from the fluctuating or heterogeneous polar metallic states, which would pave a novel route to improving thermoelectric efficiency.

There has been increasing interest in phenomena emerging from relativistic electrons in a solid, which have a potential impact on spintronics and magnetoelectrics. One example is the Rashba effect, which lifts the electron-spin degeneracy as a consequence of spin-orbit interaction under broken inversion symmetry. A high-energy-scale Rashba spin splitting is highly desirable for enhancing the coupling between electron spins and electricity relevant for spintronic functions. Here we describe the finding of a huge spin-orbit interaction effect in a polar semiconductor composed of heavy elements, BiTeI, where the bulk carriers are ruled by large Rashba-like spin splitting. The band splitting and its spin polarization obtained by spin- and angle-resolved photoemission spectroscopy are well in accord with relativistic first-principles calculations, confirming that the spin splitting is indeed derived from bulk atomic configurations. Together with the feasibility of carrier-doping control, the giant-Rashba semiconductor BiTeI possesses excellent potential for application to various spin-dependent electronic functions.

We report magnetotransport measurements on a high-mobility two-dimensional electron system at the nonmagnetic MgZnO/ZnO heterointerface showing distinct behavior for electrons with spin-up and spin-down orientations. The low-field Shubnikov-de Haas oscillations manifest alternating resistance peak heights which can be attributed to distinct scattering rates for different spin orientations. The tilt-field measurements at a half-integer filling factor reveal that the majority spins show usual diffusive behavior, i.e., peaks with the magnitude proportional to the index of the Landau level at the Fermi energy. By contrast, the minority spins develop "plateaus" with the magnitude of dissipative resistivity that is fairly independent of the Landau level index and is of the order of the zero-field resistivity.

Methods to generate spin-polarised electronic states in non-magnetic solids are strongly desired to enable all-electrical manipulation of electron spins for new quantum devices. This is generally accepted to require breaking global structural inversion symmetry. In contrast, here we present direct evidence from spin- and angle-resolved photoemission spectroscopy for a strong spin polarisation of bulk states in the centrosymmetric transition-metal dichalcogenide WSe$_2$. We show how this arises due to a lack of inversion symmetry in constituent structural units of the bulk crystal where the electronic states are localised, leading to enormous spin splittings up to $\sim\!0.5$ eV, with a spin texture that is strongly modulated in both real and momentum space. As well as providing the first experimental evidence for a recently-predicted `hidden' spin polarisation in inversion-symmetric materials, our study sheds new light on a putative spin-valley coupling in transition-metal dichalcogenides, of key importance for using these compounds in proposed valleytronic devices., Comment: 6 pages, 4 figures

BiTeI is a polar semiconductor with gigantic Rashba spin-split bands in bulk. We have investigated the effect of pressure on the electronic structure of this material via magnetotransport. Periods of Shubunikov--de Haas (SdH) oscillations originating from the spin-split outer Fermi surface and inner Fermi surface show disparate responses to pressure, while the carrier number derived from the Hall effect is unchanged with pressure. The associated parameters which characterize the spin-split band structure are strongly dependent on pressure, reflecting the pressure-induced band deformation. We find the SdH oscillations and transport response are consistent with the theoretically proposed pressure-induced band deformation leading to a topological phase transition. Our analysis suggests the critical pressure for the quantum phase transition near ${P}_{\mathrm{c}}=3.5$ GPa.

The change in the electronic structure of layered Cu${}_{x}$IrTe${}_{2}$ has been characterized by transport and spectroscopic measurements, combined with first-principles calculations. The Cu intercalation suppresses the monoclinic distortion, giving rise to the stabilization of the trigonal phase with superconductivity. Thermopower and Hall resistivity measurements suggest the multiband nature with hole and electron carriers for this system, which is masked by the predominance of the hole carriers enhanced by the interlayer hybridization in the trigonal phase. Rather than the instability of the Ir $d$ band, a subtle balance between the interlayer and intralayer Te-Te hybridizations is proposed as a main factor dominating the structural transition and the superconductivity.

Topological invariants are conventionally known to be responsible for protection of extended states against disorder. A prominent example is the presence of topologically protected extended-states in two-dimensional (2D) quantum Hall systems as well as on the surface of three-dimensional (3D) topological insulators. Distinct from such cases, here we introduce a new concept, that is, the topological protection of bound states against hybridization. This situation is shown to be realizable in a 2D quantum Hall insulator put on a 3D trivial insulator. In such a configuration, there exist topologically protected bound states, localized along the normal direction of 2D plane, in spite of hybridization with the continuum of extended states. The one-dimensional edge states are also localized along the same direction as long as their energies are within the band gap. This finding demonstrates the dual role of topological invariants, as they can also protect bound states against hybridization in a continuum., 21 pages, 7 figures

We study the magnetic susceptibility of a layered semiconductor BiTeI with giant Rashba spin splitting both theoretically and experimentally to explore its orbital magnetism. Apart from the core contributions, a large temperature-dependent diamagnetic susceptibility is observed when the Fermi energy E_F is near the crossing point of the conduction bands, while the susceptibility turns to be paramagnetic when E_F is away from it. These features are consistent with first-principles calculations, which also predict an enhanced orbital magnetic susceptibility with both positive and negative signs as a function of E_F due to band (anti)crossings. Based on these observations, we propose two mechanisms for an enhanced paramagnetic orbital susceptibility., 4 figures; added references

We investigate the two-dimensional (2D) highly spin-polarized electron accumulation layers commonly appearing near the surface of n-type polar semiconductors BiTeX (X = I, Br, and Cl) by angular-resolved photoemission spectroscopy. Due to the polarity and the strong spin-orbit interaction built in the bulk atomic configurations, the quantized conduction-band subbands show giant Rashba-type spin-splitting. The characteristic 2D confinement effect is clearly observed also in the valence-bands down to the binding energy of 4 eV. The X-dependent Rashba spin-orbit coupling is directly estimated from the observed spin-split subbands, which roughly scales with the inverse of the band-gap size in BiTeX., Comment: 15 pages 4 figures

In layered polar semiconductor BiTeI, giant Rashba-type spin-split band dispersions show up due to the crystal structure asymmetry and the strong spin-orbit interaction. Here we investigate the 3-dimensional (3D) bulk band structures of BiTeI using the bulk-sensitive $h\nu$-dependent soft x-ray angle resolved photoemission spectroscopy (SX-ARPES). The obtained band structure is shown to be well reproducible by the first-principles calculations, with huge spin splittings of ${\sim}300$ meV at the conduction-band-minimum and valence-band-maximum located in the $k_z=\pi/c$ plane. It provides the first direct experimental evidence of the 3D Rashba-type spin splitting in a bulk compound., Comment: 9 pages, 4 figures

The spin-orbit interaction affects the electronic structure of solids in various ways. Topological insulators are one example where the spin-orbit interaction leads the bulk bands to have a non-trivial topology, observable as gapless surface or edge states. Another example is the Rashba effect, which lifts the electron-spin degeneracy as a consequence of spin-orbit interaction under broken inversion symmetry. It is of particular importance to know how these two effects, i.e. the non-trivial topology of electronic states and Rashba spin splitting, interplay with each other. Here we show, through sophisticated first-principles calculations, that BiTeI, a giant bulk Rashba semiconductor, turns into a topological insulator under a reasonable pressure. This material is shown to exhibit several unique features such as, a highly pressure-tunable giant Rashba spin splitting, an unusual pressure-induced quantum phase transition, and more importantly the formation of strikingly different Dirac surface states at opposite sides of the material., Comment: 5 figures are included

We demonstrate the formation of a two-dimensional electron gas (2DEG) at the $(100)$ surface of the $5d$ transition-metal oxide KTaO$_3$. From angle-resolved photoemission, we find that quantum confinement lifts the orbital degeneracy of the bulk band structure and leads to a 2DEG composed of ladders of subband states of both light and heavy carriers. Despite the strong spin-orbit coupling, our measurements provide a direct upper bound for potential Rashba spin splitting of only $\Delta{k}_\parallel\sim\0.02$ \AA$^{-1}$ at the Fermi level. The polar nature of the KTaO$_3(100)$ surface appears to help mediate formation of the 2DEG as compared to non-polar SrTiO$_3(100)$., Comment: 5 pages, 3 figures

First-principles calculations are carried out to study the effect of electron correlations on relative structural stability, magnetism, and spin-dependent transport in ${\text{CeMnNi}}_{4}$ intermetallic compound. The correct description of Coulomb repulsion of $\text{Mn}\text{ }3d$ electrons is shown to play a crucial role in reproducing the experimentally observed cubic phase of ${\text{CeMnNi}}_{4}$ as well as its relatively high degree of transport spin polarization $(\ensuremath{\sim}66\mathrm{%})$. These are the two fundamental properties of this compound which conventional density-functional theory approaches fail to predict correctly. The reason for this failure is attributed to an extreme overdelocalization of $\text{Mn}\text{ }3d$ charges causing a strong $d\text{\ensuremath{-}}d$ hybridization between Mn and Ni atoms in the orthorhombic phase. Such an artificial hybridization, in turn, lowers the relative total energy of the orthorhombic phase with respect to the cubic one. It also leads to an incorrect carrier concentration and mobility at the Fermi level and, consequently, yields much lower degree of transport spin polarization for this nearly half-metallic compound.

Using first-principles density functional calculations, the structural, magnetic, and spin-dependent transport properties of a set of intermetallic compounds ${\mathrm{CeNi}}_{4}M$ $(M=\mathrm{Sc}\text{\ensuremath{-}}\mathrm{Co})$ are investigated. All the compounds are considered to be in the orthorhombic phase, in which a transition metal atom $M$ substitutes for one of the Ni atoms in the parent hexagonal ${\mathrm{CeNi}}_{5}$ structure. The optimized lattice constants are shown to be in good agreement with the corresponding experimental data. The volume of ${\mathrm{CeNi}}_{4}M$ turns out to decrease with changing the $M$ component from Sc to Co. Our calculations reveal that the ferromagnetic state is energetically more favorable for the compounds with $M=\mathrm{Sc}$, Mn, Fe, and Co, while for ${\mathrm{CeNi}}_{4}\mathrm{Cr}$, the structure is found to be antiferromagnetic. Except for ${\mathrm{CeNi}}_{4}\mathrm{Sc}$, the magnetism in these compounds originates mainly from $M$ atoms. The ferromagnetic coupling is mediated through the indirect $d\text{\ensuremath{-}}d$ and $d\text{\ensuremath{-}}f$ exchange interactions. The spin-dependent transport calculations show that the spin polarization in the diffusive regime is significantly higher than that in the ballistic one for these intermetallic compounds.

The manganese doped indium tin oxide (ITO) has integrated magnetics, electronics, and optical properties for next generation multifunctional devices. Our first-principles density functional theory (DFT) calculations show that the manganese atom replaces b-site indium atom, located at the second coordination shell of the interstitial oxygen in ITO. It is also found that both anti-ferromagnetic and ferromagnetic behaviors are realizable. The calculated magnetic moment of 3.95μB/Mn as well as the high transmittance of ∼80% for a 150 nm thin film of Mn doped ITO is in good agreement with the experimental data. The inclusion of on-site Coulomb repulsion corrections via DFT + U methods turns out to improve the optical behavior of the system. The optical behaviors of this system reveal its suitability for the magneto-opto-electronic applications.

We have performed a set of first-principles simulations to consider the possible phase transitions in molecular crystals of HCN under high pressure. Our calculations reveal several transition paths from the orthorhombic phase to tetragonal and then to triclinic phases. The transitions from the orthorhombic to the tetragonal phases are of the second order, whereas those from the tetragonal to the triclinic phases turn out to be of the first-order type and characterized by an abrupt decrease in volume. Our calculations show that, by adjustment of the temperature and pressure of the HCN molecular crystal, novel layered and polymeric crystals with insulating, semiconducting or metallic properties can be found. Based on our simulation results, two different crystal formation mechanisms are deduced. The stabilities of the predicted structures at ambient pressure are further assessed by performing phonon or MD simulations. In addition, the electron transport properties of the predicted polymers are obtained using the non-equilibrium Green's function technique combined with density functional theory. The results show that the polymers have metallic-like I-V characteristics.

Based on first-principles density functional calculations, a general approach for determining and analyzing the degree of spin polarization (P) in ferromagnets is presented. The approach employs the so-called tetrahedron method to evaluate the Fermi surface integrations of P in both ballistic and diffusive regimes. The validity of the method is examined by comparing the calculated P values for Fe and Ni with the experiment. The method is shown to yield highly accurate results with minimal computational effort. Within our approach, it is also possible to systematically analyze the contributions of various types of electronic states to the spin induced transport. As a case study, the transport properties of the soft-ferromagnet CeMnNi4 are investigated in order to explain the origin of the existing difference between the experimental and theoretical values of P in this intermetallic compound., 6 pages, 4 figures; to appear in Physical Review B 75 (2007)