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In-Plane Orbital Texture Switch at the Dirac Point in the Topological Insulator Bi2Se3

Topological insulators are novel macroscopic quantum-mechanical phase of matter, which hold promise for realizing some of the most exotic particles in physics as well as application towards spintronics and quantum computation. In all the known topological insulators, strong spin-orbit coupling is critical for the generation of the protected massless surface states. Consequently, a complete description of the Dirac state should include both the spin and orbital (spatial) parts of the wavefunction. For the family of materials with a single Dirac cone, theories and experiments agree qualitatively, showing the topological state has a chiral spin texture that changes handedness across the Dirac point (DP), but they differ quantitatively on how the spin is polarized. Limited existing theoretical ideas predict chiral local orbital angular momentum on the two sides of the DP. However, there have been neither direct measurements nor calculations identifying the global symmetry of the spatial wavefunction. Here we present the first results from angle-resolved photoemission experiment and first-principles calculation that both show, counter to current predictions, the in-plane orbital wavefunctions for the surface states of Bi2Se3 are asymmetric relative to the DP, switching from being tangential to the k-space constant energy surfaces above DP, to being radial to them below the DP. Because the orbital texture switch occurs exactly at the DP this effect should be intrinsic to the topological physics, constituting an essential yet missing aspect in the description of the topological Dirac state. Our results also indicate that the spin texture may be more complex than previously reported, helping to reconcile earlier conflicting spin resolved measurements.

cond-mat.mtrl-sci↗

Ferromagnetic exchange, spin-orbit coupling and spiral magnetism at the LaAlO_3/SrTiO_3 interface

The electronic properties of the polar interface between insulating oxides is a subject of great current interest. An exciting new development is the observation of robust magnetism at the interface of two non-magnetic materials LaAlO_3 (LAO) and SrTiO_3 (STO). Here we present a microscopic theory for the formation and interaction of local moments, which depends on essential features of the LAO/STO interface. We show that correlation-induced moments arise due to interfacial splitting of orbital degeneracy. We find that gate-tunable Rashba spin-orbit coupling at the interface influences the exchange interaction mediated by conduction electrons. We predict that the zero-field ground state is a long-wavelength spiral and show that its evolution in an external field accounts semi-quantitatively for torque magnetometry data. Our theory describes qualitative aspects of the scanning SQUID measurements and makes several testable predictions for future experiments.

cond-mat.str-el↗

Stabilizing isolated skyrmions at low magnetic fields exploiting vanishing magnetic anisotropy

Skyrmions are topologically protected non-collinear magnetic structures. Their stability and dynamics, arising from their topological character, have made them ideal information carriers e.g. in racetrack memories. The success of such a memory critically depends on the ability to stabilize and manipulate skyrmions at low magnetic fields. The driving force for skyrmion formation is the non-collinear Dzyaloshinskii-Moriya exchange interaction (DMI) originating from spin-orbit coupling (SOC). It competes with both the nearest neighbour Heisenberg exchange interaction and the magnetic anisotropy, which favour collinear states. While skyrmion lattices might evolve at vanishing magnetic fields, the formation of isolated skyrmions in ultra-thin films so far required the application of an external field which can be as high as several T. Here, we show that isolated skyrmions in a monolayer (ML) of Co epitaxially grown on a Ru(0001) substrate can be stabilized at magnetic fields as low as 100 mT. Even though SOC is weak in the 4d element Ru, a homochiral spin spiral ground state and isolated skyrmions could be detected and laterally resolved using a combination of tunneling and anisotropic tunneling magnetoresistance effect in spin-sensitive scanning tunneling microscopy (STM). Density functional theory (DFT) calculations confirm these chiral magnetic textures, even though the stabilizing DMI interaction is weak. We find that the key factor is the absence of magnetocristalline anisotropy in this system which enables non-collinear states to evolve in spite of weak SOC, opening up a wide choice of materials beyond 5d elements.

cond-mat.mtrl-sci↗

Competing Coulomb and electron-phonon interactions in NbS$_2$

The interplay of Coulomb and electron-phonon interactions with thermal and quantum fluctuations facilitates rich phase diagrams in two-dimensional electron systems. Layered transition metal dichalcogenides hosting charge, excitonic, spin and superconducting order form an epitomic material class in this respect. Theoretical studies of materials like NbS$_2$ have focused on the electron-phonon coupling whereas the Coulomb interaction, particularly strong in the monolayer limit, remained essentially untouched. Here, we analyze the interplay of short- and long-range Coulomb as well as electron-phonon interactions in NbS$_2$ monolayers. The combination of these interactions causes electronic correlations that are fundamentally different to what would be expected from the interaction terms separately. The fully interacting electronic spectral function resembles the non-interacting band structure but with appreciable broadening. An unexpected coexistence of strong charge and spin fluctuations puts NbS$_2$ close to spin and charge order, suggesting monolayer NbS$_2$ as a platform for atomic scale engineering of electronic quantum phases.

cond-mat.str-el↗

Vapor-Liquid-Solid Growth of Monolayer MoS2 Nanoribbons

Chemical vapor deposition (CVD) of two-dimensional (2D) materials such as monolayer MoS2 typically involves the conversion of vapor-phase precursors to a solid product in a process that may be described as a vapor-solid-solid (VSS) mode. Here, we report the first demonstration of vapor-liquid-solid (VLS) growth of monolayer MoS2 yielding highly crystalline ribbon-shaped structures with a width of a few tens of nanometers to a few micrometers. The VLS growth mode is triggered by the reaction between molybdenum oxide and sodium chloride, which results in the formation of molten Na-Mo-O droplets. These droplets mediate the growth of MoS2 ribbons in the "crawling mode" when saturated with sulfur on a crystalline substrate. Our growth yields straight and kinked ribbons with a locally well-defined orientation, reflecting the regular horizontal motion of the liquid droplets during growth. Using atomic-resolution scanning transmission electron microscopy (STEM) and second harmonic generation (SHG) microscopy, we show that the ribbons are homoepitaxially on monolayer MoS2 surface with predominantly 2H- or 3R-type stacking. These findings pave the way to novel devices with structures of mixed dimensionalities.

cond-mat.mtrl-sci↗

Non-volatile ferroelastic switching of the Verwey transition and resistivity of epitaxial Fe3O4/PMN-PT (011)

A central goal of electronics based on correlated materials or 'Mottronics' is the ability to switch between distinct collective states with a control voltage. Small changes in structure and charge density near a transition can tip the balance between competing phases, leading to dramatic changes in electronic and magnetic properties. In this work, we demonstrate that an electric field induced two-step ferroelastic switching pathway in (011) oriented 0.71Pb(Mg1/3Nb2/3)O3-0.29PbTiO3 (PMN-PT) substrates can be used to tune the Verwey metal-insulator transition in epitaxial Fe3O4 films in a stable and reversible manner. We also observe robust non-volatile resistance switching in Fe3O4 up to room temperature, driven by ferroelastic strain. These results provides a framework for realizing non-volatile and reversible tuning of order parameters coupled to lattice-strain in epitaxial oxide heterostructures over a broad range of temperatures, with potential device applications.

cond-mat.mtrl-sci↗

Superconductivity in Topological Insulator Sb2Te3 Induced by Pressure

Topological superconductivity is one of most fascinating properties of topological quantum matters that was theoretically proposed and can support Majorana Fermions at the edge state. Superconductivity was previously realized in a Cu-intercalated Bi2Se3 topological compound or a Bi2Te3 topological compound at high pressure. Here we report the discovery of superconductivity in the topological compound Sb2Te3 when pressure was applied. The crystal structure analysis results reveal that superconductivity at a low-pressure range occurs at the ambient phase. The Hall coefficient measurements indicate the change of p-type carriers at a low-pressure range within the ambient phase, into n-type at higher pressures, showing intimate relation to superconducting transition temperature. The first principle calculations based on experimental measurements of the crystal lattice show that Sb2Te3 retains its Dirac surface states within the low-pressure ambient phase where superconductivity was observed, which indicates a strong relationship between superconductivity and topology nature.

cond-mat.mtrl-sci↗

Magnetoelectric coupling in the paramagnetic state of a metal-organic framework

Although the magnetoelectric effects - the mutual control of electric polarization by magnetic fields and magnetism by electric fields, have been intensively studied in a large number of inorganic compounds and heterostructures, they have been rarely observed in organic materials. Here we demonstrate magnetoelectric coupling in a metal-organic framework [(CH3)2NH2]Mn(HCOO)3 which exhibits an order-disorder type of ferroelectricity below 185 K. The magnetic susceptibility starts to deviate from the Curie-Weiss law at the paraelectric-ferroelectric transition temperature, suggesting an enhancement of short-range magnetic correlation in the ferroelectric state. Electron spin resonance study further confirms that the magnetic state indeed changes following the ferroelectric phase transition. Inversely, the ferroelectric polarization can be improved by applying high magnetic fields. We interpret the magnetoelectric coupling in the paramagnetic state in the metal-organic framework as a consequence of the magnetoelastic effect that modifies both the superexchange interaction and the hydrogen bonding.

cond-mat.mtrl-sci↗

Oxypnictide SmFeAs(O,F) superconductor: a candidate for high-field magnet applications

The recently discovered oxypnictide superconductor SmFeAs(O,F) is the most attractive material among the Fe-based superconductors due to its highest transition temperature of 56 K and potential for high-field performance. In order to exploit this new material for superconducting applications, the knowledge and understanding of its electro-magnetic properties are needed. Recent success in fabricating epitaxial SmFeAs(O,F) thin films opens a great opportunity to explore their transport properties. Here we report on a high critical current density of over 10^5 A/cm^2 at 45 T and 4.2 K for both main field orientations, feature favourable for high-field magnet applications. Additionally, by investigating the pinning properties, we observed a dimensional crossover between the superconducting coherence length and the FeAs interlayer distance at 30-40 K, indicative of a possible intrinsic Josephson junction in SmFeAs(O,F) at low temperatures that can be employed in electronics applications such as a terahertz radiation source and a superconducting Qubit.

cond-mat.supr-con↗

Crystal, magnetic, and electronic structures, and properties of new BaMnPnF (Pn = As, Sb, Bi)

New fluoropnictides BaMnPnF with Pn = As, Sb, Bi, are synthesized by stoichiometric reaction of elements with BaF\_2. The compounds crystallize in the tetragonal P4/nmm (No. 129, Z = 2) space group, with the ZrCuSiAs-type structure, as indicated by single crystal and powder X-ray diffraction results. Electrical resistivity results indicate that Pn = As, Sb, and Bi are semiconductors with band gaps of E\_g = 0.73 eV, E\_g = 0.48 eV and E\_g = 0.003 eV, respectively. Powder neutron diffraction reveals a G-type antiferromagnetic order below T\_N = 338(1) K for Pn = As, and below T\_N = 272(1) K for Pn = Sb. Magnetic susceptibility increases with temperature above 100 K for all the materials. Density functional calculations also find semiconducting antiferromagnetic compounds with strong in-plane and weaker out-of-plane exchange coupling that may result in non-Curie Weiss behavior above T\_N. There is strong covalency between Mn and pnictogen elements. The ordered magnetic moments are 3.65(5) μB/Mn for Pn = As, and 3.66(3) μB/Mn for Pn = Sb at 4 K, as refined from neutron diffraction experiments.

cond-mat.str-el↗

Large Linear Magnetoresistance and Shubnikov-de Hass Oscillations in Single Crystals of YPdBi Heusler Topological Insulators

We report the observation of a large linear magnetoresistance (MR) and Shubnikov-de Hass (SdH) quantum oscillations in single crystals of YPdBi Heusler topological insulators. Owning to the successfully obtained the high-quality YPdBi single crystals, large non-saturating linear MR of as high as 350% at 5K and over 120% at 300 K under a moderate magnetic field of 7 T is observed. In addition to the large, field-linear MR, the samples exhibit pronounced SdH quantum oscillations at low temperature. Analysis of the SdH data manifests that the high-mobility bulk electron carriers dominate the magnetotransport and are responsible for the observed large linear MR in YPdBi crystals. These findings imply that the Heusler-based topological insulators have superiorities for investigating the novel quantum transport properties and developing the potential applications.

cond-mat.mtrl-sci↗

Orientation Dependent Thermal Conductance in Single-Layer MoS2

We investigate the thermal conductivity in the armchair and zigzag MoS$_{2}$ nanoribbons, by combining the non-equilibrium Green's function approach and the first-principles method. A strong orientation dependence is observed in the thermal conductivity. Particularly, the thermal conductivity for the armchair MoS$_{2}$ nanoribbon is about 673.6 Wm$^{-1}$K$^{-1}$ in the armchair nanoribbon, and 841.1 Wm$^{-1}$K$^{-1}$ in the zigzag nanoribbon at room temperature. By calculating the Caroli transmission, we disclose the underlying mechanism for this strong orientation dependence to be the fewer phonon transport channels in the armchair MoS$_{2}$ nanoribbon in the frequency range of [150, 200] {cm$^{-1}$}. Through the scaling of the phonon dispersion, we further illustrate that the thermal conductivity calculated for the MoS$_{2}$ nanoribbon is esentially in consistent with the superior thermal conductivity found for graphene.

cond-mat.mtrl-sci↗

High Performance Molybdenum Disulfide Amorphous Silicon Heterojunction Photodetector

One important use of layered semiconductors such as molybdenum disulfide (MoS2) could be in making novel heterojunction devices leading to functionalities unachievable using conventional semiconductors. Here we demonstrate an ultrafast metal-semiconductor-metal heterojunction photodetector, made of MoS2 and amorphous silicon (a-Si), with rise and fall times of about 0.3 ms. This is more than an order of magnitude improvement over response times of conventional a-Si (~5 ms) and best reported MoS2 devices (~50 ms). The van-der-waals heterojunction presented here yields a high photoresponsivity of 210 mA/W at green light-the wavelength used in commercial imaging systems. This responsivity is 4X larger than that of the best MoS2 devices, and 2X larger than that of commercial a-Si devices. The 10X improvement in speed with high photoresponsivity provides a potential solution to a decades-long problem for thin film imagers and could find applications in large area electronics such as biomedical imaging and x-ray fluoroscopy.

cond-mat.mtrl-sci↗

Precisely aligned graphene grown on hexagonal boron nitride by catalyst free chemical vapor deposition

To grow precisely aligned graphene on h-BN without metal catalyst is extremely important, which allows for intriguing physical properties and devices of graphene/h-BN hetero-structure to be studied in a controllable manner. In this report, such hetero-structures were fabricated and investigated by atomic resolution scanning probe microscopy. Moirre patterns are observed and the sensitivity of moirre interferometry proves that the graphene grains can align precisely with the underlying h-BN lattice within an error of less than 0.05 degree. The occurrence of moirre pattern clearly indicates that the graphene locks into h-BN via van der Waals epitaxy with its interfacial stress greatly released. It is worthy to note that the edges of the graphene grains are primarily oriented along the armchair direction. The field effect mobility in such graphene flakes exceeds 20,000 cm2/V.s at ambient condition. This work opens the door of atomic engineering of graphene on h-BN, and sheds light on fundamental research as well as electronic applications based on graphene/h-BN hetero-structure.

cond-mat.mtrl-sci↗

Efficient Gate-tunable light-emitting device made of defective boron nitride nanotubes: from ultraviolet to the visible

Boron nitride is a promising material for nanotechnology applications due to its two-dimensional graphene-like, insulating, and highly-resistant structure. Recently it has received a lot of attention as a substrate to grow and isolate graphene as well as for its intrinsic UV lasing response. Similar to carbon, one-dimensional boron nitride nanotubes (BNNTs) have been theoretically predicted and later synthesised. Here we use first principles simulations to unambiguously demonstrate that i) BN nanotubes inherit the highly efficient UV luminescence of hexagonal BN; ii) the application of an external perpendicular field closes the electronic gap keeping the UV lasing with lower yield; iii) defects in BNNTS are responsible for tunable light emission from the UV to the visible controlled by a transverse electric field (TEF). Our present findings pave the road towards optoelectronic applications of BN-nanotube-based devices that are simple to implement because they do not require any special doping or complex growth.

cond-mat.mtrl-sci↗

Charge transport in lithium peroxide: Relevance for rechargeable metal-air batteries

The mechanisms and efficiency of charge transport in lithium peroxide (Li2O2) are key factors in understanding the performance of non-aqueous Li-air batteries. Towards revealing these mechanisms, here we use first-principles calculations to predict the concentrations and mobilities of charge carriers and intrinsic defects in Li2O2 as a function of cell voltage. Our calculations reveal that changes in the charge state of O2 dimers controls the defect chemistry and conductivity of Li2O2. Negative lithium vacancies (missing Li+) and small hole polarons are identified as the dominant charge carriers. The electronic conductivity associated with polaron hopping (5 x 10-20 S/cm) is comparable to the ionic conductivity arising from the migration of Li-ions (4 x 10-19 S/cm), suggesting that charge transport in Li2O2 occurs through a mixture of ionic and polaronic contributions. These data indicate that the bulk regions of crystalline Li2O2 are insulating, with appreciable charge transport occurring only at moderately high charging potentials that drive partial delithiation. The implications of limited charge transport on discharge and recharge mechanisms are discussed, and a two-stage charging process linking charge transport, discharge product morphology, and overpotentials is described. We conclude that achieving both high discharge capacities and efficient charging will depend upon access to alternative mechanisms that bypass bulk charge transport. More generally, we describe how the presence of a species that can change charge state - e.g., O2 dimers in alkaline metal-based peroxides - may impact rechargeability in metal-air batteries.

cond-mat.mtrl-sci↗

Spin-polarized electronic structure of the core-shell ZnO/ZnO:Mn nanowires probed by x-ray absorption and emission spectroscopy

The combination of x-ray spectroscopy methods complemented with theoretical analysis unravels the coexistence of paramagnetic and antiferromagnetic phases in the Zn_0.9Mn_0.1O shell deposited onto array of wurtzite ZnO nanowires. The shell is crystalline with orientation toward the ZnO growth axis, as demonstrated by X-ray linear dichroism. EXAFS analysis confirmed that more than 90% of Mn atoms substituted Zn in the shell while fraction of secondary phases was below 10%. The value of manganese spin magnetic moment was estimated from the Mn Kβ X-ray emission spectroscopy to be 4.3μB which is close to the theoretical value for substitutional Mn_Zn. However the analysis of L_2,3 x-ray magnetic circular dichroism data showed paramagnetic behaviour with saturated spin magnetic moment value of 1.95μB as determined directly from the spin sum rule. After quantitative analysis employing atomic multiplet simulations such difference was explained by a coexistence of paramagnetic phase and local antiferromagnetic coupling of Mn magnetic moments. Finally, spin-polarized electron density of states was probed by the spin-resolved Mn K-edge XANES spectroscopy and consequently analyzed by band structure calculations.

cond-mat.mtrl-sci↗

Approaches to modelling irradiation-induced processes in transmission electron microscopy

The recent progress in high-resolution transmission electron microscopy (HRTEM) has given rise to the possibility of in situ observations of nanostructure transformations and chemical reactions induced by electron irradiation. In this article we briefly summarise experimental observations and discuss in detail atomistic modelling of irradiation-induced processes in HRTEM, as well as mechanisms of such processes recognised due to modelling. Accurate molecular dynamics (MD) techniques based on first principles or tight-binding models are employed in the analysis of single irradiation-induced events, and classical MD simulations are combined with a kinetic Monte Carlo algorithm to simulate continuous irradiation of nanomaterials. It has been shown that sulphur-terminated graphene nanoribbons are formed inside carbon nanotubes as a result of an irradiation-selective chemical reaction. The process of fullerene formation in HRTEM during continuous electron irradiation of a small graphene flake has been simulated, and mechanisms driving this transformation analysed.

cond-mat.mtrl-sci↗