Prediction and observation of an antiferromagnetic topological insulator.

Magnetic topological insulators are narrow-gap semiconductor materials that combine non-trivial band topology and magnetic order1. Unlike their nonmagnetic counterparts, magnetic topological insulators may have some of the surfaces gapped, which enables a number of exotic phenomena that have potential applications in spintronics1, such as the quantum anomalous Hall effect2 and chiral Majorana fermions3. So far, magnetic topological insulators have only been created by means of doping nonmagnetic topological insulators with 3d transition-metal elements; however, such an approach leads to strongly inhomogeneous magnetic4 and electronic5 properties of these materials, restricting the observation of important effects to very low temperatures2,3. An intrinsic magnetic topological insulator-a stoichiometric well ordered magnetic compound-could be an ideal solution to these problems, but no such material has been observed so far. Here we predict by ab initio calculations and further confirm using various experimental techniques the realization of an antiferromagnetic topological insulator in the layered van der Waals compound MnBi2Te4. The antiferromagnetic ordering  that MnBi2Te4  shows makes it invariant with respect to the combination of the time-reversal and primitive-lattice translation symmetries, giving rise to a ℤ2 topological classification; ℤ2 = 1 for MnBi2Te4, confirming its topologically nontrivial nature. Our experiments indicate that the symmetry-breaking (0001) surface of MnBi2Te4 exhibits a large bandgap in the topological surface state. We expect this property to eventually enable the observation of a number of fundamental phenomena, among them quantized magnetoelectric coupling6-8 and axion electrodynamics9,10. Other exotic phenomena could become accessible at much higher temperatures than those reached so far, such as the quantum anomalous Hall effect2 and chiral Majorana fermions3.

Origin of the Magnetic Exciton in the van der Waals Antiferromagnet NiPS_{3}.

An ultrasharp photoluminescence line intimately related to antiferromagnetic order has been found in NiPS_{3}, a correlated van der Waals material, opening prospects for magneto-optical coupling schemes and spintronic applications. Here we unambiguously clarify the singlet origin of this excitation, confirming its roots in the spin structure. Based on a comprehensive investigation of the electronic structure using angle-resolved photoemission and q-dependent electron energy loss spectroscopy as experimental tools we develop, in a first step, an adequate theoretical understanding using density functional theory (DFT). In a second step the DFT is used as input for a dedicated multiplet theory by which we achieve excellent agreement with available multiplet spectroscopy. Our Letter connects the understanding of the electronic structure and of optical processes in NiPS_{3} and related materials as a prerequisite for further progress of the field.

Orbital Complexity in Intrinsic Magnetic Topological Insulators MnBi_{4}Te_{7} and MnBi_{6}Te_{10}.

Using angle-resolved photoelectron spectroscopy (ARPES), we investigate the surface electronic structure of the magnetic van der Waals compounds MnBi_{4}Te_{7} and MnBi_{6}Te_{10}, the n=1 and 2 members of a modular (Bi_{2}Te_{3})_{n}(MnBi_{2}Te_{4}) series, which have attracted recent interest as intrinsic magnetic topological insulators. Combining circular dichroic, spin-resolved and photon-energy-dependent ARPES measurements with calculations based on density functional theory, we unveil complex momentum-dependent orbital and spin textures in the surface electronic structure and disentangle topological from trivial surface bands. We find that the Dirac-cone dispersion of the topologial surface state is strongly perturbed by hybridization with valence-band states for Bi_{2}Te_{3}-terminated surfaces but remains preserved for MnBi_{2}Te_{4}-terminated surfaces. Our results firmly establish the topologically nontrivial nature of these magnetic van der Waals materials and indicate that the possibility of realizing a quantized anomalous Hall conductivity depends on surface termination.

Unraveling the Nature of Magnetism of the 5d

We report electron spin resonance (ESR) spectroscopy results on the double perovskite Ba_{2}YIrO_{6}. On general grounds, this material is expected to be nonmagnetic due to the strong coupling of the spin and orbital momenta of Ir^{5+} (5d^{4}) ions. However, controversial experimental reports on either strong antiferromagnetism with static order at low temperatures or just a weakly paramagnetic behavior have triggered a discussion on the breakdown of the generally accepted scenario of the strongly spin-orbit coupled ground states in the 5d^{4} iridates and the emergence of a novel exotic magnetic state. Our data evidence that the magnetism of the studied material is solely due to a few percent of Ir^{4+} and Ir^{6+} magnetic defects while the regular Ir^{5+} sites remain nonmagnetic. Remarkably, the defect Ir^{6+} species manifest magnetic correlations in the ESR spectra at T≲20 K, suggesting a long-range character of superexchange in the double perovskites as proposed by recent theories.

Induction Mapping of the 3D-Modulated Spin Texture of Skyrmions in Thin Helimagnets.

Envisaged applications of Skyrmions in magnetic memory and logic devices crucially depend on the stability and mobility of these topologically nontrivial magnetic textures in thin films. We present for the first time quantitative maps of the magnetic induction that provide evidence for a 3D modulation of the Skyrmionic spin texture. The projected in-plane magnetic induction maps as determined from in-line and off-axis electron holography carry the clear signature of Bloch Skyrmions. However, the magnitude of this induction is much smaller than the values expected for homogeneous Bloch Skyrmions that extend throughout the thickness of the film. This finding can only be understood if the underlying spin textures are modulated along the out-of-plane z direction. The projection of (the in-plane magnetic induction of) helices is further found to exhibit thickness-dependent lateral shifts, which show that this z modulation is accompanied by an (in-plane) modulation along the x and y directions.

Magnetization relaxation in the single-ion magnet DySc2N@C80: quantum tunneling, magnetic dilution, and unconventional temperature dependence.

Relaxation of magnetization in endohedral metallofullerenes DySc2N@C80 is studied at different temperatures, in different magnetic fields, and in different molecular arrangements. Magnetization behavior and relaxation are analyzed for powder sample, and for DySc2N@C80 diluted in non-magnetic fullerene Lu3N@C80, adsorbed in voids of a metal-organic framework, and dispersed in a polymer. The magnetic field dependence and zero-field relaxation are also studied for single-crystals of DySc2N@C80 co-crystallized with Ni(ii) octaethylporphyrin, as well as for the single crystal diluted with Lu3N@C80. Landau-Zener theory is applied to analyze quantum tunneling of magnetization in the crystals. The field dependence of relaxation rates revealed a dramatic dependence of the zero-field tunneling resonance width on the dilution and is explained with the help of an analysis of dipolar field distributions. AC magnetometry is used then to get access to the relaxation of magnetization in a broader temperature range, from 2 to 87 K. Finally, a theoretical framework describing the spin dynamics with dissipation is proposed to study magnetization relaxation phenomena in single molecule magnets.

Evidence for a Field-Induced Quantum Spin Liquid in α-RuCl_{3}.

We report a ^{35}Cl nuclear magnetic resonance study in the honeycomb lattice α-RuCl_{3}, a material that has been suggested to potentially realize a Kitaev quantum spin liquid (QSL) ground state. Our results provide direct evidence that α-RuCl_{3} exhibits a magnetic-field-induced QSL. For fields larger than ∼10 T, a spin gap opens up while resonance lines remain sharp, evidencing that spins are quantum disordered and locally fluctuating. The spin gap increases linearly with an increasing magnetic field, reaching ∼50 K at 15 T, and is nearly isotropic with respect to the field direction. The unusual rapid increase of the spin gap with increasing field and its isotropic nature are incompatible with conventional magnetic ordering and, in particular, exclude that the ground state is a fully polarized ferromagnet. The presence of such a field-induced gapped QSL phase has indeed been predicted in the Kitaev model.

Orbital-driven nematicity in FeSe.

A fundamental and unconventional characteristic of superconductivity in iron-based materials is that it occurs in the vicinity of two other instabilities. In addition to a tendency towards magnetic order, these Fe-based systems have a propensity for nematic ordering: a lowering of the rotational symmetry while time-reversal invariance is preserved. Setting the stage for superconductivity, it is heavily debated whether the nematic symmetry breaking is driven by lattice, orbital or spin degrees of freedom. Here, we report a very clear splitting of NMR resonance lines in FeSe at Tnem = 91 K, far above the superconducting Tc of 9.3 K. The splitting occurs for magnetic fields perpendicular to the Fe planes and has the temperature dependence of a Landau-type order parameter. Spin-lattice relaxation rates are not affected at Tnem, which unequivocally establishes orbital degrees of freedom as driving the nematic order. We demonstrate that superconductivity competes with the emerging nematicity.

J_{eff} Description of the Honeycomb Mott Insulator α-RuCl_{3}.

Novel ground states might be realized in honeycomb lattices with strong spin-orbit coupling. Here we study the electronic structure of α-RuCl_{3}, in which the Ru ions are in a d^{5} configuration and form a honeycomb lattice, by angle-resolved photoemission, x-ray photoemission, and electron energy loss spectroscopy supported by density functional theory and multiplet calculations. We find that α-RuCl_{3} is a Mott insulator with significant spin-orbit coupling, whose low energy electronic structure is naturally mapped onto J_{eff} states. This makes α-RuCl_{3} a promising candidate for the realization of Kitaev physics. Relevant electronic parameters such as the Hubbard energy U, the crystal field splitting 10 Dq, and the charge transfer energy Δ are evaluated.

Complex Field-Induced States in Linarite PbCuSO4(OH)2 with a Variety of High-Order Exotic Spin-Density Wave States.

Low-temperature neutron diffraction and NMR studies of field-induced phases in linarite are presented for magnetic fields H∥b axis. A two-step spin-flop transition is observed, as well as a transition transforming a helical magnetic ground state into an unusual magnetic phase with sine-wave-modulated moments ∥H. An effective J[over ˜]_{1}-J[over ˜]_{2} single-chain model with a magnetization-dependent frustration ratio α_{eff}=-J[over ˜]_{2}/J[over ˜]_{1} is proposed. The latter is governed by skew interchain couplings and shifted to the vicinity of the ferromagnetic critical point. It explains qualitatively the observation of a rich variety of exotic longitudinal collinear spin-density wave, SDW_{p}, states (9≥p≥2).

Unusual Dirac Fermions on the Surface of a Noncentrosymmetric α-BiPd Superconductor.

Combining multiple emergent correlated properties such as superconductivity and magnetism within the topological matrix can have exceptional consequences in garnering new and exotic physics. Here, we study the topological surface states from a noncentrosymmetric α-BiPd superconductor by employing angle-resolved photoemission spectroscopy and first-principles calculations. We observe that the Dirac surface states of this system have several interesting and unusual properties, compared to other topological surface states. The surface state is strongly anisotropic and the in-plane Fermi velocity varies rigorously on rotating the crystal about the y axis. Moreover, it acquires an unusual band gap as a function of k_{y}, possibly due to hybridization with bulk bands, detected upon varying the excitation energy. The coexistence of all the functional properties in addition to the unusual surface state characteristics make this an interesting material.

Anisotropic Particle-Hole Excitations in Black Phosphorus.

We report on the energy- and momentum-resolved optical response of black phosphorus (BP) in its bulk form. Along the armchair direction of the puckered layers, we find a highly dispersive mode that is strongly suppressed in the perpendicular (zigzag) direction. This mode emerges out of the single-particle continuum for finite values of momentum and is therefore interpreted as an exciton. We argue that this exciton, which has already been predicted theoretically for phosphorene-the monolayer form of BP-can be detected by conventional optical spectroscopy in the two-dimensional case and might pave the way for optoelectronic applications of this emerging material.

Mutual Independence of Critical Temperature and Superfluid Density under Pressure in Optimally Electron-Doped Superconducting LaFeAsO(1-x)F(x).

The superconducting properties of LaFeAsO(1-x)F(x) under conditions of optimal electron doping are investigated upon the application of external pressure up to ∼23 kbar. Measurements of muon-spin spectroscopy and dc magnetometry evidence a clear mutual independence between the critical temperature T(c) and the low-temperature saturation value for the ratio n(s)/m(*) (superfluid density over effective band mass of Cooper pairs). Remarkably, a dramatic increase of ∼30% is reported for n(s)/m(*) at the maximum pressure value while T(c) is substantially unaffected in the whole accessed experimental window. We argue and demonstrate that the explanation for the observed results must take the effect of nonmagnetic impurities on multiband superconductivity into account. In particular, the unique possibility to modify the ratio between intraband and interband scattering rates by acting on structural parameters while keeping the amount of chemical disorder constant is a striking result of our proposed model.

(pi, pi) electronic order in iron arsenide superconductors.

The distribution of valence electrons in metals usually follows the symmetry of the underlying ionic lattice. Modulations of this distribution often occur when those electrons are not stable with respect to a new electronic order, such as spin or charge density waves. Electron density waves have been observed in many families of superconductors, and are often considered to be essential for superconductivity to exist. Recent measurements seem to show that the properties of the iron pnictides are in good agreement with band structure calculations that do not include additional ordering, implying no relation between density waves and superconductivity in these materials. Here we report that the electronic structure of Ba(1-x)K(x)Fe(2)As(2) is in sharp disagreement with those band structure calculations, and instead reveals a reconstruction characterized by a (pi, pi) wavevector. This electronic order coexists with superconductivity and persists up to room temperature (300 K).

Thin film growth of Fe-based superconductors: from fundamental properties to functional devices. A comparative review.

Fe-based superconductors bridge a gap between MgB2 and the cuprate high temperature superconductors as they exhibit multiband character and transition temperatures up to around 55 K. Investigating Fe-based superconductors thus promises answers to fundamental questions concerning the Cooper pairing mechanism, competition between magnetic and superconducting phases, and a wide variety of electronic correlation effects. The question addressed in this review is, however, is this new class of superconductors also a promising candidate for technical applications? Superconducting film-based technologies range from high-current and high-field applications for energy production and storage to sensor development for communication and security issues and have to meet relevant needs of today's society and that of the future. In this review we will highlight and discuss selected key issues for Fe-based superconducting thin film applications. We initially focus our discussion on the understanding of physical properties and actual problems in film fabrication based on a comparison of different observations made in the last few years. Subsequently we address the potential for technological applications according to the current situation.

Quasiballistic transport of Dirac fermions in a Bi2Se3 nanowire.

Quantum coherent transport of surface states in a mesoscopic nanowire of the three-dimensional topological insulator Bi(2}Se(3) is studied in the weak-disorder limit. At very low temperatures, many harmonics are evidenced in the Fourier transform of Aharonov-Bohm oscillations, revealing the long phase coherence length of spin-chiral Dirac fermions. Remarkably, from their exponential temperature dependence, we infer an unusual 1/T power law for the phase coherence length L(φ)(T). This decoherence is typical for quasiballistic fermions weakly coupled to their environment.

Spin pseudogap in Ni-doped SrCuO2.

The S=1/2 spin chain material SrCuO2 doped with 1% S=1 Ni impurities is studied by inelastic neutron scattering. At low temperatures, the spectrum shows a pseudogap Δ≈8 meV, absent in the parent compound, and not related to any structural phase transition. The pseudogap is shown to be a generic feature of quantum spin chains with dilute defects. A simple model based on this idea quantitatively accounts for the experimental data measured in the temperature range from 2 to 300 K, and allows us to represent the momentum-integrated dynamic structure factor in a universal scaling form.

Retro-fitting an older (S)TEM with two Cs aberration correctors for 80 kV and 60 kV operation.

For the characterization of light materials using transmission electron microscopy, a low electron acceleration voltage of 80 kV or even 60 kV is attractive due to reduced beam damage to the specimen. The concomitant reduction in resolving power of the microscope can be restored when using spherical aberration (C(s) ) correctors, which for the most part are only available in the latest and most expensive microscopes. Here, we show that upgrading of existing TEMs is an attractive and cost-effective alternative. We report on the low-voltage performance on graphitic material of a JEOL JEM-2010F built in the early 1990s and retro-fitted with a conventional imaging C(s) corrector and a probe C(s) corrector. The performance data show C(s) retro-fitted instruments can compete very favourably against more modern state-of-the-art instruments in both conventional imaging (TEM) and scanning (STEM) modes.

Graphene at high bias: cracking, layer by layer sublimation, and fusing.

Graphene and few-layer graphene at high bias expose a wealth of phenomena due to the high temperatures reached. With in situ transmission electron microscopy, we observe directly how the current modifies the structure, and vice versa. In some samples, cracks propagate from the edges of the flakes, leading to the formation of narrow constrictions or to nanometer spaced gaps after breakdown. In other samples, we find layer-by-layer evaporation of few-layer graphene, which could be exploited for the controlled production of single layer graphene from multilayered samples. Surprisingly, we even find that two pieces of graphene that overlap can heal out at high bias and form one continuous sheet. These findings open up new avenues to structure graphene for specific device applications.

Magnetic frustration, phase competition, and the magnetoelectric effect in NdFe3(BO3)4.

We present an element selective resonant magnetic x-ray scattering study of NdFe3(BO3)4 as a function of temperature and applied magnetic field. Our measurements show that the magnetic order of the Nd sublattice is induced by the Fe spin order. When a magnetic field is applied parallel to the hexagonal basal plane, the helicoidal spin order is suppressed and a collinear ordering, where the moments are forced to align in a direction perpendicular to the applied magnetic field, is stabilized. This result excludes a noncollinear spin order as the origin of the magnetically induced electric polarization in this compound. Instead our data imply that magnetic frustration results in a phase competition, which is the origin of the magnetoelectric response.