Spin-Reorientation-Driven Linear Magnetoelectric Effect in Topological Antiferromagnet Cu_{3}TeO_{6}.

The search for new materials for energy-efficient electronic devices has gained unprecedented importance. Among the various classes of magnetic materials driving this search are antiferromagnets, magnetoelectrics, and systems with topological spin excitations. Cu_{3}TeO_{6} is a material that belongs to all three of these classes. Combining static electric polarization and magnetic torque measurements with phenomenological simulations we demonstrate that magnetic-field-induced spin reorientation needs to be taken into account to understand the linear magnetoelectric effect in Cu_{3}TeO_{6}. Our calculations reveal that the magnetic field pushes the system from the nonpolar ground state to the polar magnetic structures. However, nonpolar structures only weakly differing from the obtained polar ones exist due to the weak effect that the field-induced breaking of some symmetries has on the calculated structures. Among those symmetries is the PT (1[over ¯]^{'}) symmetry, preserved for Dirac points found in Cu_{3}TeO_{6}. Our findings establish Cu_{3}TeO_{6} as a promising playground to study the interplay of spintronics-related phenomena.

Origin of Subgap States in Normal-Insulator-Superconductor van der Waals Heterostructures.

Superconductivity in van der Waals materials, such as NbSe2 and TaS2, is fundamentally novel due to the effects of dimensionality, crystal symmetries, and strong spin-orbit coupling. In this work, we perform tunnel spectroscopy on NbSe2 by utilizing MoS2 or hexagonal boron nitride (hBN) as a tunnel barrier. We observe subgap excitations and probe their origin by studying various heterostructure designs. We show that the edge of NbSe2 hosts many defect states, which strongly couple to the superconductor and form Andreev bound states. Furthermore, by isolating the NbSe2 edge we show that the subgap states are ubiquitous in MoS2 tunnel barriers but absent in hBN tunnel barriers, suggesting defects in MoS2 as their origin. Their magnetic nature reveals a singlet- or a doublet-type ground state, and based on nearly vanishing g factors or avoided crossings of subgap excitations, we highlight the role of strong spin-orbit coupling.

Room-temperature skyrmion phase in bulk Cu2OSeO3 under high pressures.

A skyrmion state in a noncentrosymmetric helimagnet displays topologically protected spin textures with profound technological implications for high-density information storage, ultrafast spintronics, and effective microwave devices. Usually, its equilibrium state in a bulk helimagnet occurs only over a very restricted magnetic field-temperature phase space and often in the low-temperature region near the magnetic transition temperature Tc We have expanded and enhanced the skyrmion phase region from the small range of 55 to 58.5 K to 5 to 300 K in single-crystalline Cu2OSeO3 by pressures up to 42.1 GPa through a series of phase transitions from the cubic P213, through orthorhombic P212121 and monoclinic P21, and finally to the triclinic P1 phase, using our newly developed ultrasensitive high-pressure magnetization technique. The results are in agreement with our Ginzburg-Landau free energy analyses, showing that pressures tend to stabilize the skyrmion states and at higher temperatures. The observations also indicate that the skyrmion state can be achieved at higher temperatures in various crystal symmetries, suggesting the insensitivity of skyrmions to the underlying crystal lattices and thus the possible more ubiquitous presence of skyrmions in helimagnets.

van der Waals π Josephson Junctions.

Proximity-induced superconductivity in a ferromagnet can induce Cooper pairs with a finite center-of-mass momentum and stabilize Josephson junctions (JJs) with π phase difference in superconductor-ferromagnet-superconductor heterostructures. The emergence of two-dimensional layered superconducting and magnetic materials promises a new platform for realizing π JJs with atomically sharp interfaces. Here we demonstrate a thickness-driven 0-π transition in JJs made of NbSe2 (an Ising superconductor) and Cr2Ge2Te6 (a ferromagnetic semiconductor). By systematically increasing the Cr2Ge2Te6 weak link thickness, we observe a vanishing supercurrent at a critical thickness of ∼8 nm, followed by a re-entrant supercurrent. Near the critical thickness, we further observe unusual supercurrent interference patterns with vanishing critical current around zero in-plane magnetic field. They signify the formation of 0-π JJs (with both 0 and π regions), likely induced by the nanoscale magnetic domains in Cr2Ge2Te6.

Axial-Bonding-Driven Dimensionality Effect on the Charge-Density Wave in NbSe2.

2H-NbSe2 is a prototypical charge-density-wave (CDW) system, exhibiting such a symmetry-breaking quantum ground state in its bulk and down to a single-atomic-layer limit. However, how this state depends on dimensionality and what governs the dimensionality effect remain controversial. Here, we experimentally demonstrate a robust 3 × 3 CDW phase in both freestanding and substrate-supported bilayer NbSe2, far above the bulk transition temperature. We exclude environmental effects and reveal a strong temperature and thickness dependence of Raman intensity from an axially vibrating A1g phonon mode, involving Se ions. Using first-principles calculations, we show that these result from a delicate but profound competition between the intra- and interlayer bonding formed between Se-pz orbitals. Our results suggest the crucial role of Se out-of-plane displacement in driving the CDW distortion, revealing the Se-dominated dimensionality effect and establishing a new perspective on the chemical bonding and mechanical stability in layered CDW materials.

Ultrafast dynamics in (TaSe4)2I triggered by valence and core-level excitation.

Dimensionality plays a key role in the emergence of ordered phases, such as charge density-waves (CDW), which can couple to, and modulate, the topological properties of matter. In this work, we study the out-of-equilibrium dynamics of the paradigmatic quasi-one-dimensional material (TaSe4)2I, which exhibits a transition into an incommensurate CDW phase when cooled to just below room temperature, namely at TCDW = 263 K. We make use of both optical laser and free-electron laser (FEL) based time-resolved spectroscopies in order to study the effect of a selective excitation on the normal-state and on the CDW phases by probing the near-infrared/visible optical properties both along and perpendicularly to the direction of the CDW, where the system is metallic and insulating, respectively. Excitation of the core-levels by ultrashort X-ray FEL pulses at 47 eV and 119 eV induces reflectivity transients resembling those recorded when only exciting the valence band of the compound - by near-infrared pulses at 1.55 eV - in the case of the insulating sub-system. Conversely, the metallic sub-system displays relaxation dynamics which depend on the energy of photo-excitation. Moreover, excitation of the CDW amplitude mode is recorded only for excitation at a low-photon-energy. This fact suggests that the coupling of light to ordered states of matter can predominantly be achieved when directly injecting delocalized carriers in the valence band, rather than localized excitations in the core levels. Complementing this, table-top experiments allow us to prove the quasi-unidirectional nature of the CDW phase in (TaSe4)2I, whose fingerprints are detected along its c-axis only. Our results provide new insights into the symmetry of the ordered phase of (TaSe4)2I perturbed by a selective excitation, and suggest a novel approach based on complementary table-top and FEL spectroscopies for the study of complex materials.

Microwave Spectroscopy of the Low-Temperature Skyrmion State in Cu_{2}OSeO_{3}.

In the cubic chiral magnet Cu_{2}OSeO_{3} a low-temperature skyrmion state (LTS) and a concomitant tilted conical state are observed for magnetic fields parallel to ⟨100⟩. Here, we report on the dynamic resonances of these novel magnetic states. After promoting the nucleation of the LTS by means of field cycling, we apply broadband microwave spectroscopy in two experimental geometries that provide either predominantly in-plane or out-of-plane excitation. By comparing the results to linear spin-wave theory, we clearly identify resonant modes associated with the tilted conical state, the gyrational and breathing modes associated with the LTS, as well as the hybridization of the breathing mode with a dark octupole gyration mode mediated by the magnetocrystalline anisotropies. Most intriguingly, our findings suggest that under decreasing fields the hexagonal skyrmion lattice becomes unstable with respect to an oblique deformation, reflected in the formation of elongated skyrmions.

Reciprocal space tomography of 3D skyrmion lattice order in a chiral magnet.

It is commonly assumed that surfaces modify the properties of stable materials within the top few atomic layers of a bulk specimen only. Exploiting the polarization dependence of resonant elastic X-ray scattering to go beyond conventional diffraction and imaging techniques, we have determined the depth dependence of the full 3D spin structure of skyrmions-that is, topologically nontrivial whirls of the magnetization-below the surface of a bulk sample of Cu2OSeO3 We found that the skyrmions change exponentially from pure Néel- to pure Bloch-twisting over a distance of several hundred nanometers between the surface and the bulk, respectively. Though qualitatively consistent with theory, the strength of the Néel-twisting at the surface and the length scale of the variation observed experimentally exceed material-specific modeling substantially. In view of the exceptionally complete quantitative theoretical account of the magnetic rigidities and associated static and dynamic properties of skyrmions in Cu2OSeO3 and related materials, we conclude that subtle changes of the materials properties must exist at distances up to several hundred atomic layers into the bulk, which originate in the presence of the surface. This has far-reaching implications for the creation of skyrmions in surface-dominated systems and identifies, more generally, surface-induced gradual variations deep within a bulk material and their impact on tailored functionalities as an unchartered scientific territory.

Charge transfer enhanced magnetic correlations in type-II multiferroic Co3TeO6.

Magnetic structure of the Co ions in monoclinic Co3TeO6 in the antiferroelectric state at 16 K has been determined by neutron powder together with single-crystal diffractions. The indices of the magnetic reflections that appear at the incommensurate positions were determined by diffractions from a single crystal, which allow to uniquely identify the magnetic modulation vector. There are two crystallographically distinct Co layers. Magnetic incommensurability appears in the Co spins in the layers comprising zig-zag chains, with a magnetic modulation vector of (0.357, 0.103, 0.121) at 3 K but changes to (0.4439, 0, 0.137) at 16 K, while the Co ions in the honeycomb webs form a collinear antiferromagnetic structure. Thermal reduction rate of the Co moments in the honeycomb webs was found to be much smaller than those in the zigzag chains. Shifting of large amounts of electronic charge into the Co─O bonds in the honeycomb webs on warming is used to understand the behavior.

Archetypal Soft-Mode-Driven Antipolar Transition in Francisite Cu_{3}Bi(SeO_{3})_{2}O_{2}Cl.

Model materials are precious test cases for elementary theories and provide building blocks for the understanding of more complex cases. Here, we describe the lattice dynamics of the structural phase transition in francisite Cu_{3}Bi(SeO_{3})_{2}O_{2}Cl at 115 K and show that it provides a rare archetype of a transition driven by a soft antipolar phonon mode. In the high-symmetry phase at high temperatures, the soft mode is found at (0,0,0.5) at the Brillouin zone boundary and is measured by inelastic x-ray scattering and thermal diffuse scattering. In the low-symmetry phase, this soft-mode is folded back onto the center of the Brillouin zone as a result of the doubling of the unit cell, and appears as a fully symmetric mode that can be tracked by Raman spectroscopy. On both sides of the transition, the mode energy squared follows a linear behavior over a large temperature range. First-principles calculations reveal that, surprisingly, the flat phonon band calculated for the high-symmetry phase seems incompatible with the displacive character found experimentally. We discuss this unusual behavior in the context of an ideal Kittel model of an antiferroelectric transition.

Band Filling and Cross Quantum Capacitance in Ion-Gated Semiconducting Transition Metal Dichalcogenide Monolayers.

Ionic liquid gated field-effect transistors (FETs) based on semiconducting transition metal dichalcogenides (TMDs) are used to study a rich variety of extremely interesting physical phenomena, but important aspects of how charge carriers are accumulated in these systems are not understood. We address these issues by means of a systematic experimental study of transport in monolayer MoSe2 and WSe2 as a function of magnetic field and gate voltage, exploring accumulated densities of carriers ranging from approximately 1014 cm-2 holes in the valence band to 4 × 1014 cm-2 electrons in the conduction band. We identify the conditions when the chemical potential enters different valleys in the monolayer band structure (the K and Q valley in the conduction band and the two spin-split K-valleys in the valence band) and find that an independent electron picture describes the occupation of states well. Unexpectedly, however, the experiments show very large changes in the device capacitance when multiple valleys are occupied that are not at all compatible with the commonly expected quantum capacitance contribution of these systems, CQ = e2/ (dµ/dn). A theoretical analysis of all terms responsible for the total capacitance shows that under general conditions a term is present besides the usual quantum capacitance, which becomes important for very small distances between the capacitor plates. This term, which we call cross quantum capacitance, originates from screening of the electric field generated by charges on one plate from charges sitting on the other plate. The effect is negligible in normal capacitors but large in ionic liquid FETs because of the atomic proximity between the ions in the gate and the accumulated charges on the TMD, and it accounts for all our experimental observations. Our findings therefore reveal an important contribution to the capacitance of physical systems that had been virtually entirely neglected until now.

An unusual continuous paramagnetic-limited superconducting phase transition in 2D NbSe 2.

Time reversal and spatial inversion are two key symmetries for conventional Bardeen-Cooper-Schrieffer (BCS) superconductivity 1 . Breaking inversion symmetry can lead to mixed-parity Cooper pairing and unconventional superconducting properties1-5. Two-dimensional (2D) NbSe2 has emerged as a new non-centrosymmetric superconductor with the unique out-of-plane or Ising spin-orbit coupling (SOC)6-9. Here we report the observation of an unusual continuous paramagnetic-limited superconductor-normal metal transition in 2D NbSe2. Using tunelling spectroscopy under high in-plane magnetic fields, we observe a continuous closing of the superconducting gap at the upper critical field at low temperatures, in stark contrast to the abrupt first-order transition observed in BCS thin-film superconductors10-12. The paramagnetic-limited continuous transition arises from a large spin susceptibility of the superconducting phase due to the Ising SOC. The result is further supported by self-consistent mean-field calculations based on the ab initio band structure of 2D NbSe2. Our findings establish 2D NbSe2 as a promising platform to explore novel spin-dependent superconducting phenomena and device concepts 1 , such as equal-spin Andreev reflection 13 and topological superconductivity14-16.

Semiconducting van der Waals Interfaces as Artificial Semiconductors.

Recent technical progress demonstrates the possibility of stacking together virtually any combination of atomically thin crystals of van der Waals bonded compounds to form new types of heterostructures and interfaces. As a result, there is the need to understand at a quantitative level how the interfacial properties are determined by the properties of the constituent 2D materials. We address this problem by studying the transport and optoelectronic response of two different interfaces based on transition-metal dichalcogenide monolayers, namely WSe2-MoSe2 and WSe2-MoS2. By exploiting the spectroscopic capabilities of ionic liquid gated transistors, we show how the conduction and valence bands of the individual monolayers determine the bands of the interface, and we establish quantitatively (directly from the measurements) the energetic alignment of the bands in the different materials as well as the magnitude of the interfacial band gap. Photoluminescence and photocurrent measurements allow us to conclude that the band gap of the WSe2-MoSe2 interface is direct in k space, whereas the gap of WSe2/MoS2 is indirect. For WSe2/MoSe2, we detect the light emitted from the decay of interlayer excitons and determine experimentally their binding energy using the values of the interfacial band gap extracted from transport measurements. The technique that we employed to reach this conclusion demonstrates a rather-general strategy for characterizing quantitatively the interfacial properties in terms of the properties of the constituent atomic layers. The results presented here further illustrate how van der Waals interfaces of two distinct 2D semiconducting materials are composite systems that truly behave as artificial semiconductors, the properties of which can be deterministically defined by the selection of the appropriate constituent semiconducting monolayers.

Spin-Resolved Electronic Response to the Phase Transition in MoTe_{2}.

The semimetal MoTe_{2} is studied by spin- and angle-resolved photoemission spectroscopy across the centrosymmetry-breaking structural transition temperature of the bulk. A three-dimensional spin-texture is observed in the bulk Fermi surface in the low temperature, noncentrosymmetric phase that is consistent with first-principles calculations. The spin texture and two types of surface Fermi arc are not completely suppressed above the bulk transition temperature. The lifetimes of quasiparticles forming the Fermi arcs depend on thermal history and lengthen considerably upon cooling toward the bulk structural transition. The results indicate that a new form of polar instability exists near the surface when the bulk is largely in a centrosymmetric phase.

Microscopic Origin of the Valley Hall Effect in Transition Metal Dichalcogenides Revealed by Wavelength-Dependent Mapping.

The band structure of many semiconducting monolayer transition metal dichalcogenides (TMDs) possesses two degenerate valleys with equal and opposite Berry curvature. It has been predicted that, when illuminated with circularly polarized light, interband transitions generate an unbalanced nonequilibrium population of electrons and holes in these valleys, resulting in a finite Hall voltage at zero magnetic field when a current flows through the system. This is the so-called valley Hall effect that has recently been observed experimentally. Here, we show that this effect is mediated by photogenerated neutral excitons and charged trions and not by interband transitions generating independent electrons and holes. We further demonstrate an experimental strategy, based on wavelength dependent spatial mapping of the Hall voltage, which allows the exciton and trion contributions to the valley Hall effect to be discriminated in the measurement. These results represent a significant step forward in our understanding of the microscopic origin of photoinduced valley Hall effect in semiconducting transition metal dichalcogenides and demonstrate experimentally that composite quasi-particles, such as trions, can also possess a finite Berry curvature.

Heuristic Description of Magnetoelectricity of Cu2OSeO3.

CuO2SeO3 is an insulating material that hosts topologically nontrivial spin whirls, so-called skyrmions, and exhibits magnetoelectric coupling allowing to manipulate these skyrmions by means of electric fields. We report magnetic force microscopy imaging of the real-space spin structure on the surface of a bulk single crystal of CuO2SeO3. Based on measurements of the electric polarization using Kelvin-probe force microscopy, we develop a heuristic description of the magnetoelectric properties in CuO2SeO3. The model successfully describes the dependency of the electric polarization on the magnetization in all magnetically modulated phases.

Time-resolved ARPES at LACUS: Band Structure and Ultrafast Electron Dynamics of Solids.

The manipulation of the electronic properties of solids by light is an exciting goal, which requires knowledge of the electronic structure with energy, momentum and temporal resolution. Time- and angle-resolved photoemission spectroscopy (tr-ARPES) is the most direct probe of the effects of an optical excitation on the band structure of a material. In particular, tr-ARPES in the extreme ultraviolet (VUV) range gives access to the ultrafast dynamics over the entire Brillouin zone. VUV tr-ARPES experiments can now be performed at the ASTRA (ARPES Spectrometer for Time-Resolved Applications) end station of Harmonium, at LACUS. Its capabilities are illustrated by measurements of the ultrafast electronic response of ZrSiTe, a novel topological semimetal characterized by linearly dispersing states located at the Brillouin zone boundary.

Gate Tuning of Electronic Phase Transitions in Two-Dimensional NbSe_{2}.

Recent experimental advances in atomically thin transition metal dichalcogenide (TMD) metals have unveiled a range of interesting phenomena including the coexistence of charge-density-wave (CDW) order and superconductivity down to the monolayer limit. The atomic thickness of two-dimensional (2D) TMD metals also opens up the possibility for control of these electronic phase transitions by electrostatic gating. Here, we demonstrate reversible tuning of superconductivity and CDW order in model 2D TMD metal NbSe_{2} by an ionic liquid gate. A variation up to ∼50% in the superconducting transition temperature has been observed. Both superconductivity and CDW order can be strengthened (weakened) by increasing (reducing) the carrier density in 2D NbSe_{2}. The doping dependence of these phase transitions can be understood as driven by a varying electron-phonon coupling strength induced by the gate-modulated carrier density and the electronic density of states near the Fermi surface.

Snapshots of cooperative atomic motions in the optical suppression of charge density waves.

Macroscopic quantum phenomena such as high-temperature superconductivity, colossal magnetoresistance, ferrimagnetism and ferromagnetism arise from a delicate balance of different interactions among electrons, phonons and spins on the nanoscale. The study of the interplay among these various degrees of freedom in strongly coupled electron-lattice systems is thus crucial to their understanding and for optimizing their properties. Charge-density-wave (CDW) materials, with their inherent modulation of the electron density and associated periodic lattice distortion, represent ideal model systems for the study of such highly cooperative phenomena. With femtosecond time-resolved techniques, it is possible to observe these interactions directly by abruptly perturbing the electronic distribution while keeping track of energy relaxation pathways and coupling strengths among the different subsystems. Numerous time-resolved experiments have been performed on CDWs, probing the dynamics of the electronic subsystem. However, the dynamics of the periodic lattice distortion have been only indirectly inferred. Here we provide direct atomic-level information on the structural dynamics by using femtosecond electron diffraction to study the quasi two-dimensional CDW system 1T-TaS(2). Effectively, we have directly observed the atomic motions that result from the optically induced change in the electronic spatial distribution. The periodic lattice distortion, which has an amplitude of ∼0.1 Å, is suppressed by about 20% on a timescale (∼250 femtoseconds) comparable to half the period of the corresponding collective mode. These highly cooperative, electronically driven atomic motions are accompanied by a rapid electron-phonon energy transfer (∼350 femtoseconds) and are followed by fast recovery of the CDW (∼4 picoseconds). The degree of cooperativity in the observed structural dynamics is remarkable and illustrates the importance of obtaining atomic-level perspectives of the processes directing the physics of strongly correlated systems.

Electrostatically induced superconductivity at the surface of WS2.

We investigate transport through ionic liquid gated field effect transistors (FETs) based on exfoliated crystals of semiconducting WS2. Upon electron accumulation, at surface densities close to, or just larger than, 10(14) cm(-2), transport exhibits metallic behavior with the surface resistivity decreasing pronouncedly upon cooling. A detailed characterization as a function of temperature and magnetic field clearly shows the occurrence of a gate-induced superconducting transition below a critical temperature Tc ≈ 4 K, a finding that represents the first demonstration of superconductivity in tungsten-based semiconducting transition metal dichalcogenides. We investigate the nature of superconductivity and find significant inhomogeneity, originating from the local detaching of the frozen ionic liquid from the WS2 surface. Despite the inhomogeneity, we find that in all cases where a fully developed zero resistance state is observed, different properties of the devices exhibit a behavior characteristic of a Berezinskii-Kosterlitz-Thouless transition, as it could be expected in view of the two-dimensional nature of the electrostatically accumulated electron system.