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Non-collinear magnetic skyrmion lattices provide novel magnonic functionalities due to their topological magnon bands and asymmetric dispersion relations. Magnon excitations with intermediate wavelengths comparable to inter-skyrmion distances are particularly interesting but largely unexplored so far due to experimental challenges. Here, we report the detection of such magnons with wavevectors q $\simeq$ 48 rad/um in the metastable skyrmion lattice phase of the bulk chiral magnet Cu$_2$OSeO$_3$ using micro-focused Brillouin light scattering microscopy. Thanks to its high sensitivity and broad bandwidth we resolved various excitation modes of a single skyrmion lattice domain over a wide magnetic field regime. Besides the known modes with dipole character, quantitative comparison of frequencies and spectral weights to theoretical predictions enabled the identification of a quadrupole mode and observation of signatures which we attribute to a decupole and a sextupole mode. Our combined experimental and theoretical work highlights that skyrmionic phases allow for the design of magnonic devices exploiting topological magnon bands.

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 (ME) 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 $PT$ ($\overline{1}'$) 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., Comment: 6 pages, 4 figures

The transition-metal dichalcogenide tantalum disulphide (1$T$-TaS$_2$) hosts a commensurate charge density wave (CCDW) at temperatures below 165~K where it also becomes insulating. The low temperature CCDW phase can be driven into a metastable "mosaic" phase by means of either laser or voltage pulses which shows a large density of CDW domain walls as well as a closing of the electronic band gap. The exact origins of this pulse-induced metallic mosaic are not yet fully understood. Here, using scanning tunneling microscopy and spectroscopy (STM/STS), we observe the occurrence of such a metallic mosaic phase on the surface of TaS$_2$ without prior pulse excitation over continuous areas larger than $100 \times 100$~nm$^2$ and macroscopic areas on the millimetre scale. We attribute the appearance of the mosaic phase to the presence of surface defects which cause the formation of the characteristic dense domain wall network. Based on our STM measurements, we further argue how the appearance of the metallic behaviour in the mosaic phase could be explained by local stacking differences of the top layer. Thus, we provide a potential avenue to explain the origin of the pulse induced mosaic phase., Comment: 10 pages, 8 figures, under review at Physical Review Materials

Superconductivity in van der Waals materials, such as NbSe$_{2}$ and TaS$_{2}$, is fundamentally novel due to the effects of dimensionality, crystal symmetries, and strong spin-orbit coupling. In this work we perform tunnel spectroscopy on NbSe$_{2}$ by utilizing MoS$_{2}$ 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 NbSe$_{2}$ hosts many defect states, which strongly couple to the superconductor and form Andreev bound states. Furthermore, by isolating the NbSe$_{2}$ edge we show that the subgap states are ubiquitous in MoS$_{2}$ tunnel barriers, but absent in hBN tunnel barriers, suggesting defects in MoS$_{2}$ as their origin. Their magnetic nature reveals a singlet or a doublet type ground state and based on nearly vanishing g-factors or avoided-crossing of subgap excitations we highlight the role of strong spin-orbit coupling., Comment: 16 pages, 7 figures. Includes Supporting Information

The ultra-quantum limit is achieved when a magnetic field confines an electron gas in its lowest spin-polarised Landau level. Here we show that in this limit, electron doped ZrTe$_5$ shows a metal-insulator transition followed by a sign change of the Hall and Seebeck effects at low temperature. We attribute this transition to a magnetic freeze-out of charge carriers on the ionised impurities. The reduction of the charge carrier density gives way to an anomalous Hall response of the spin-polarised electrons. This behaviour, at odds with the usual magnetic freeze-out scenario, occurs in this Dirac metal because of its tiny Fermi energy, extremely narrow band gap and a large $g$-factor. We discuss the different possible sources (intrinsic or extrinsic) for this anomalous Hall contribution., Comment: 14 pages, 4 figures

In this work, we study the out-of-equilibrium dynamics of the paradigmatic quasi-one-dimensional material (TaSe$_4$)$_2$I, that exhibits a transition into an incommensurate CDW phase when cooled just below room temperature, namely at T$_{\rm{CDW}} $= 263 K. We make use of both optical laser and free-electron laser (FEL) based time-resolved spectroscopies in order to study the effect of a selective excitation on the normal-state and on the CDW phases, by probing the near-infrared/visible optical properties both along and perpendicularly to the direction of the CDW, where the system is metallic and insulating, respectively. Excitation of the core-levels by ultrashort X-ray FEL pulses at 47 eV and 119 eV induces reflectivity transients resembling those recorded when only exciting the valence band of the compound - by near-infrared pulses at 1.55 eV - in the case of the insulating sub-system. Conversely, the metallic sub-system displays a relaxation dynamics which depends on the energy of photo-excitation. Moreover, excitation of the CDW amplitude mode is recorded only for excitation at low-photon-energy. This fact suggests that the coupling of light to ordered states of matter can predominantly be achieved when directly injecting delocalized carriers in the valence band, rather than localized excitations in the core levels. On a complementary side, table-top experiments allow us to prove the quasi-unidirectional nature of the CDW phase in (TaSe$_4$)$_2$I, whose fingerprints are detected along its $c$-axis only. Our results provide new insights on the symmetry of the ordered phase of (TaSe$_4$)$_2$I perturbed by a selective excitation, and suggest a novel approach based on complementary table-top and FEL spectroscopies for the study of complex materials., Comment: 24 pages, 7 figures

Proximity-induced superconductivity in a ferromagnet can induce Cooper pairs with a finite center-of-mass momentum. The resultant spatially modulated superconducting order parameter is able to stabilize Josephson junctions (JJs) with pi phase difference in superconductor-ferromagnet heterostructures and realize 'quiet' phase qubits. The emergence of two-dimensional (2D) layered superconducting and magnetic materials promises a new platform for realizing pi JJs with atomically sharp interfaces by van der Waals stacking. Here we demonstrate a thickness-driven 0-pi transition in JJs made of NbSe2 (an Ising superconductor) with a Cr2Ge2Te6 (a ferromagnetic semiconductor) weak link. By systematically varying the Cr2Ge2Te6 thickness, we observe a vanishing supercurrent at a critical thickness around 8 nm, followed by a re-entrant supercurrent upon further increase in thickness. 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-pi JJs (with both 0 and pi regions) likely induced by the nanoscale magnetic domains in Cr2Ge2Te6. Our work highlights the potential of van der Waals superconductor-ferromagnet heterostructures for the explorations of unconventional superconductivity and superconducting electronics., Comment: none

Co$_{1/3}$NbS$_2$ is the magnetic intercalate of 2H-NbS$_2$ where electronic itinerant and magnetic properties strongly influence each other throughout the phase diagram. Here we report the first angle-resolved photoelectron spectroscopy (ARPES) study in Co$_{1/3}$NbS$_2$. The observed electronic structure seemingly resembles the one of the parent material 2H-NbS$_2$, with the shift in Fermi energy of 0.5 eV accounting for the charge transfer of approximately two electrons from each Co ion into the NbS$_2$ layers. However, we observe significant departures from the 2H-NbS$_2$ rigid band picture: Entirely unrelated to the 2H-NbS$_2$ electronic structure, a shallow electronic band is found crossing the Fermi level near the boundary of the first Brillouin zone of the superstructure imposed by the intercalation. The evolution of the experimental spectra upon varying the incident photon energy suggests the Co origin of this band. Second, the Nb bonding band, found deeply submerged below the Fermi level at the $\Gamma$ point, indicates the interlayer-hybridization being very much amplified by intercalation, with Co magnetic ions probably acting as covalent bridges between NbS$_2$ layers. The strong hybridization between conducting and magnetic degrees of freedom suggests dealing with strongly correlated electron system where the interlayer coupling plays an exquisite role., Comment: 22 pages, 20 figures

Fermi surfaces, three-dimensional (3D) abstract interfaces that define the occupied energies of electrons in a solid, are important for characterizing and predicting the thermal, electrical, magnetic, and optical properties of crystalline metals and semiconductors [1]. Angle-resolved photoemission spectroscopy (ARPES) is the only technique directly probing the Fermi surface by measuring the Fermi momenta (kF) from energy and angular distribution of photoelectrons dislodged by monochromatic light [2]. Existing electron analyzers are able to determine a number of kF-vectors simultaneously, but current technical limitations prohibit a direct high-resolution 3D Fermi surface mapping. As a result, no such datasets exist, strongly limiting our knowledge about the Fermi surfaces and restricting a detailed comparison with the widely available nowadays calculated 3D Fermi surfaces. Here we show that using a simpler instrumentation, based on the Fourier electron optics combined with a retardation field of the detector, it is possible to perform 3D-mapping within a very short time interval and with very high resolution. We present the first detailed experimental 3D Fermi surface recorded in the full Brillouin zone along the kz-direction as well as other experimental results featuring multiple advantages of our technique. In combination with various light sources, including synchrotron radiation, our methodology and instrumentation offer new opportunities for high-resolution ARPES in the physical and life sciences., Comment: 14 pages, 4 figures

Crystalline defects can modify quantum interactions in solids, causing unintuitive, even favourable, properties such as quantum Hall effect or superconducting vortex pinning. Here we present another example of this notion - an unexpected unidirectional Kondo scattering in single crystals of 2H-NbS2. This manifests as a pronounced low-temperature enhancement in the out-of-plane resistivity and thermopower below 40 K, hidden for the in-plane charge transport. The anomaly can be suppressed by the c-axis-oriented magnetic field, but is unaffected by field applied along the planes. The magnetic moments originate from layers of 1T-NbS2, which inevitably form during the growth, undergoing a charge-density-wave reconstruction with each superlattice cell (David-star-shaped cluster of Nb atoms) hosting a localised spin. Our results demonstrate the unique and highly anisotropic response of a spontaneously formed Kondo lattice heterostructure, intercalated in a layered conductor., Comment: 44 pages, including the article, 5 figures, and Supplementary Information (6 notes, 9 figures, and 1 table)

Vector-chiral (VC) antiferromagnetism is a spiral-like ordering of spins which may allow ferroelectricity to occur due to loss of space inversion symmetry. In this paper we report direct experimental observation of ferroelectricity in the VC phase of $\beta$-TeVO$_4$, a frustrated spin chain system with pronounced magnetic anisotropy and a rich phase diagram. Saturation polarization is proportional to neutron scattering intensities that correspond to the VC magnetic reflection. This implies that inverse Dzyaloshinskii-Moriya mechanism is responsible for driving electric polarization. Linear magnetoelectric coupling is absent, however an unprecedented dependence of electric coercive field on applied magnetic field reveals a novel way of manipulating multiferroic information., Comment: submitted to PRB Letter, 7 pages, 4 figures

The Dzyaloshinskii-Moriya interaction (DMI) has an impact on excited spin waves in the chiral magnet Cu$_2$OSeO$_3$ by means of introducing asymmetry on their dispersion relations. The confined eigenmodes of a chiral magnet are hence no longer the conventional standing spin waves. Here we report a combined experimental and micromagnetic modeling study by broadband microwave spectroscopy we observe confined spin waves up to eleventh order in bulk Cu$_2$OSeO$_3$ in the field-polarized state. In micromagnetic simulations we find similarly rich spectra. They indicate the simultaneous excitation of both dipole- and exchange-dominated spin waves with wavelengths down to (47.2 $\pm$ 0.05) nm attributed to the exchange interaction modulation. Our results suggest DMI to be effective to create exchange spin waves in a bulk sample without the challenging nanofabrication and thereby to explore their scattering with noncollinear spin textures.

Cu$_2$OSeO$_3$ is an insulating skyrmion-host material with a magnetoelectric coupling giving rise to an electric polarization with a characteristic dependence on the magnetic field $\vec H$. We report magnetic force microscopy imaging of the helical real-space spin structure on the surface of a bulk single crystal of Cu$_2$OSeO$_3$. In the presence of a magnetic field, the helimagnetic order in general reorients and acquires a homogeneous component of the magnetization, resulting in a conical arrangement at larger fields. We investigate this reorientation process at a temperature of 10~K for fields close to the crystallographic $\langle 110\rangle$ direction that involves a phase transition at $H_{c1}$. Experimental evidence is presented for the formation of magnetic domains in real space as well as for the microscopic origin of relaxation events that accompany the reorientation process. In addition, the electric polarization is measured by means of Kelvin-probe force microscopy. We show that the characteristic field dependency of the electric polarization originates in this helimagnetic reorientation process. Our experimental results are well described by an effective Landau theory previously invoked for MnSi, that captures the competition between magnetocrystalline anisotropies and Zeeman energy.

We experimentally study the tunability of the cooperativity in coupled spin--cavity systems by changing the magnetic state of the spin system via an external control parameter. As model system, we use the skyrmion host material Cu$_2$OSeO$_3$ coupled to a microwave cavity resonator. In the different magnetic phases we measure a dispersive coupling between the resonator and the magnon modes and model our results by using the input--output formalism. Our results show a strong tunability of the normalized coupling rate by magnetic field, allowing us to change the magnon--photon cooperativity from 1 to 60 at the phase boundaries of the skyrmion lattice state.

Superconductivity and magnetism are generally incompatible because of the opposing requirement on electron spin alignment. When combined, they produce a multitude of fascinating phenomena, including unconventional superconductivity and topological superconductivity. The emergence of two-dimensional (2D)layered superconducting and magnetic materials that can form nanoscale junctions with atomically sharp interfaces presents an ideal laboratory to explore new phenomena from coexisting superconductivity and magnetic ordering. Here we report tunneling spectroscopy under an in-plane magnetic field of superconductor-ferromagnet-superconductor (S/F/S) tunnel junctions that are made of 2D Ising superconductor NbSe2 and ferromagnetic insulator CrBr3. We observe nearly 100% tunneling anisotropic magnetoresistance (AMR), that is, difference in tunnel resistance upon changing magnetization direction from out-of-plane to inplane. The giant tunneling AMR is induced by superconductivity, particularly, a result of interfacial magnetic exchange coupling and spin-dependent quasiparticle scattering. We also observe an intriguing magnetic hysteresis effect in superconducting gap energy and quasiparticle scattering rate with a critical temperature that is 2 K below the superconducting transition temperature. Our study paves the path for exploring superconducting spintronic and unconventional superconductivity in van der Waals heterostructures., Comment: None

Tantalum diselenide (TaSe$_{2}$) is a metallic transition metal dichalcogenide whose equilibrium structure and vibrational behavior strongly depends on temperature and thickness, including the emergence of charge density wave (CDW) states at very low T. In this work, observed modes for mono- and bi-layer are described across several spectral regions and com-pared to the bulk ones. Such modes, including an experimentally observed forbidden Raman mode and low frequency CDW modes, are then matched to corresponding density functional theory (DFT) predicted vibrations, to unveil their inner working. The excellent match between experimental and computational results justifies the presented vibrational visualizations of these modes. Additional support is provided by experimental phonons seen in Raman spectra as a function of temperature and thickness. These results highlight the importance of understanding interlayer interactions and their effects on mode behaviors., Comment: arXiv admin note: substantial text overlap with arXiv:2005.11350

In the cubic chiral magnet Cu2OSeO3 a low-temperature skyrmion state (LTS) and a concomitant tilted conical state are observed for magnetic fields parallel to <100>. In this work, 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.

We report magnetic properties of a 3d$^9$ (Cu$^{2+}$) magnetic insulator Cu2OSO4 measured on both powder and single crystal. The magnetic atoms of this compound form layers, whose geometry can be described either as a system of chains coupled through dimers or as a Kagom\'e lattice where every 3rd spin is replaced by a dimer. Specific heat and DC-susceptibility show a magnetic transition at 20 K, which is also confirmed by neutron scattering. Magnetic entropy extracted from the specific heat data is consistent with a $S=1/2$ degree of freedom per Cu$^{2+}$, and so is the effective moment extracted from DC-susceptibility. The ground state has been identified by means of neutron diffraction on both powder and single crystal and corresponds to a $\sim120$ degree spin structure in which ferromagnetic intra-dimer alignment results in a net ferrimagnetic moment. No evidence is found for a change in lattice symmetry down to 2 K. Our results suggest that \sample \ represents a new type of model lattice with frustrated interactions where interplay between magnetic order, thermal and quantum fluctuations can be explored., Comment: Published in Physical Review B

$\beta$-TeVO$_4$ is a frustrated spin 1/2 zig-zag chain system,where spin-density-wave (SDW), vector chiral (VC)and an exotic dynamic spin-stripe phase compete at low temperatures. Here we use torque magnetometry to study the anisotropy of these phases in magnetic fields of up to 5 T. Our results show that the magnetic-field-induced spin reorientation occurs in the SDW and in the spin stripe phases for $\mu_0 H \geq 2$~T. The observed spin reorientation is a new element of the anisotropic phase diagram for the field directions in the $ac$ and $a^*b$ crystallographic planes. The presented results should help establishing the model of anisotropic magnetic interactions, which are responsible for the formation of complex magnetic phases in $\beta$-TeVO$_4$ and similar quantum systems., Comment: Accepted for publication in Physical Review B

Applying elastic deformation can tune a material physical properties locally and reversibly. Spatially modulated lattice deformation can create a bandgap gradient, favouring photo-generated charge separation and collection in optoelectronic devices. These advantages are hindered by the maximum elastic strain that a material can withstand before breaking. Nanomaterials derived by exfoliating transition metal dichalcogenides TMDs are an ideal playground for elastic deformation, as they can sustain large elastic strains, up to a few percent. However, exfoliable TMDs with highly strain-tunable properties have proven challenging for researchers to identify. We investigated 1T-ZrS2 and 1T-ZrSe2, exfoliable semiconductors with large bandgaps. Under compressive deformation, both TMDs dramatically change their physical properties. 1T-ZrSe2 undergoes a reversible transformation into an exotic three-dimensional lattice, with a semiconductor-to-metal transition. In ZrS2, the irreversible transformation between two different layered structures is accompanied by a sudden 14 % bandgap reduction. These results establish that Zr-based TMDs are an optimal strain-tunable platform for spatially textured bandgaps, with a strong potential for novel optoelectronic devices and light harvesting.

Metallic transition metal dichalcogenides like tantalum diselenide (TaSe$_{2}$) exhibit exciting behaviors at low temperatures, including the emergence of charge density wave (CDW) states. In this work, density functional theory (DFT) is used to investigate how structural, electronic, and Raman spectral properties of the CDW configuration change as a function of thickness. Such findings highlight the influence of dimensionality change (from 2D to 3D) and van der Waals (vdW) interactions on the system properties. The vdW effect is most strongly present in bulk TaSe$_{2}$ in the spectral range 165 cm$^{-1}$ to 215 cm$^{-1}$. The phonons seen in the experimental Raman spectra are compared with the results calculated from the DFT models as a function of temperature and layer number. The matching of data and calculations substantiates the model's description of the CDW structural formation as a function of thickness, which is shown in depth for 1L through 6L systems. These results highlight the importance of understanding interlayer interactions, which are pervasive in many quantum phenomena involving two-dimensional confinement., Comment: 6 figures, 28 pages

The discovery of the anomalous Hall effect (AHE) in bulk metallic antiferromagnets (AFMs) motivates the search of the same phenomenon in two-dimensional (2D) systems, where a quantized anomalous Hall conductance can in principle be observed. Here, we present experiments on micro-fabricated devices based on Co$_{1/3}$NbS$_2$, a layered AFM that was recently found to exhibit AHE in bulk crystals below the N\'eel temperature T$_N$ = 29 K. Transport measurements reveal a pronounced resistivity anisotropy, indicating that upon lowering temperature the electronic coupling between individual atomic layers is increasingly suppressed. The experiments also show an extremely large anomalous Hall conductivity of approximately 400 S/cm, more than one order of magnitude larger than in the bulk, which demonstrates the importance of studying the AHE in small exfoliated crystals, less affected by crystalline defects. Interestingly, the corresponding anomalous Hall conductance, when normalized to the number of contributing atomic planes, is $\sim \, 0.6 \; e^2/h$ per layer, approaching the value expected for the quantized anomalous Hall effect. The observed strong anisotropy of transport and the very large anomalous Hall conductance per layer make the properties of Co$_{1/3}$NbS$_2$ compatible with the presence of partially filled topologically non-trivial 2D bands originating from the magnetic superstructure of the antiferromagnetic state. Isolating atomically thin layers of this material and controlling their charge density may therefore provide a viable route to reveal the occurrence of the quantized AHE in a 2D AFM.

A skyrmion state in a non-centrosymmetric 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 55-58.5 K to 5-300 K in single-crystalline Cu2OSeO3 by pressures up to 42.1 GPa through a series of phase transitions from the cubic P2(_1)3, through orthorhombic P2(_1)2(_1)2(_1) and monoclinic P2(_1), 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., Comment: 22 pages, 5 figures and 3 supplementary figures

Two-dimensional transition metal dichalcogenides (TMDs) have been attracting significant interest due to a range of properties, such as layer-dependent inversion symmetry, valley-contrasted Berry curvatures, and strong spin-orbit coupling (SOC). Of particular interest is niobium diselenide (NbSe2), whose superconducting state in few-layer samples is profoundly affected by an unusual type of SOC called Ising SOC. Combined with the reduced dimensionality, the latter stabilizes the superconducting state against magnetic fields up to ~35 T and could lead to other exotic properties such as nodal and crystalline topological superconductivity. Here, we report transport measurements of few-layer NbSe$_2$ under in-plane external magnetic fields, revealing an unexpected two-fold rotational symmetry of the superconducting state. In contrast to the three-fold symmetry of the lattice, we observe that the magnetoresistance and critical field exhibit a two-fold oscillation with respect to an applied in-plane magnetic field. We find similar two-fold oscillations deep inside the superconducting state in differential conductance measurements on NbSe$_2$/CrBr$_3$ superconductor-magnet junctions. In both cases, the anisotropy vanishes in the normal state, demonstrating that it is an intrinsic property of the superconducting phase. We attribute the behavior to the mixing between two closely competing pairing instabilities, namely, the conventional s-wave instability typical of bulk NbSe$_2$ and an unconventional d- or p-wave channel that emerges in few-layer NbSe2. Our results thus demonstrate the unconventional character of the pairing interaction in a few-layer TMD, opening a new avenue to search for exotic superconductivity in this family of 2D materials., Comment: 19 pages, 4 figures plus supplementary material

Transition-metal dichalcogenides (TMDs) are layered compounds that support many electronic phases, including various charge density waves, superconducting, and Mott insulating states. Their intercalation with magnetic ions introduces magnetic sublayers, which strongly influence the coupling between host layers, and feature various magnetic states adjustable by external means. Co$_{1/3}$NbS$_2$ hosts a particularly sensitive magnetic subsystem with the lowest magnetic ordering temperature in the family of magnetically intercalated TMDs, and the only one where the complete suppression of magnetic order under pressure has been recently suggested. By combining the results of several experimental methods, electronic ab initio calculations, and modeling, we develop insights into the mechanisms of electric transport, magnetic ordering, and their interaction in this compound. The elastic neutron scattering is used to directly follow the evolution of the antiferromagnetic order parameter with pressure and temperature. Our results unambiguously disclose the complete suppression of the observed magnetic order around 1.7 GPa. We delve into possible mechanisms of magnetic order suppression under pressure, highlighting the role of magnetic frustrations indicated by magnetic susceptibility measurements and ab-initio calculations. Electronic conduction anisotropy is measured in the wide temperature and pressure range. Here we show that the transport in directions along and perpendicular to layers respond differently to the appearance of magnetic ordering or the application of the hydrostatic pressure. We propose the 'spin-valve' mechanism where the intercalated Co ions act as spin-selective electrical transport bridges between host layers. The mechanism applies to various magnetic states and can be extended to other magnetically intercalated TMDs., Comment: 36 pages, 19 figures

Two-dimensional (2D) materials have become a fertile playground for the exploration and manipulation of novel collective electronic states. Recent experiments have unveiled a variety of robust 2D orders in highly-crystalline materials ranging from magnetism to ferroelectricity and from superconductivity to charge density wave (CDW) instability. The latter, in particular, appears in diverse patterns even within the same family of materials with isoelectronic species. Furthermore, how they evolve with dimensionality has so far remained elusive. Here we propose a general framework that provides a unfied picture of CDW ordering in the 2H polytype of four isoelectronic transition metal dichalcogenides 2H-MX$_2$ (M=Nb, Ta and X=S, Se). We first show experimentally that whilst NbSe$_2$ exhibits a strongly enhanced CDW order in the 2D limit, the opposite trend exists for TaSe$_2$ and TaS$_2$, with CDW being entirely absent in NbS$_2$ from its bulk to the monolayer. Such distinct behaviours are then demonstrated to be the result of a subtle, yet profound, competition between three factors: ionic charge transfer, electron-phonon coupling, and the spreading extension of the electronic wave functions. Despite its simplicity, our approach can, in essence, be applied to other quasi-2D materials to account for their CDW response at different thicknesses, thereby shedding new light on this intriguing quantum phenomenon and its underlying mechanisms.

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 MoSe$_2$ and WSe$_2$ as a function of magnetic field and gate voltage, exploring accumulated densities of carriers ranging from approximately 10$^{14}$ cm$^{-2}$ holes in the valence band to 4x10$^{14}$ 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, $\textit{C}$$_Q$=$\textit{e}^2$/(d$\mu$/d$\textit{n}$). This unexpected behavior is attributed to the presence of a cross quantum capacitance, which originates from screening of the electric field generated by charges on one plate from charges sitting on the other plate. Our findings therefore reveal an important contribution to the capacitance of physical systems that had been virtually entirely neglected until now. (short abstract due to size limitations - full abstract in the manuscript), Comment: 5 figures

Layered transition metal dichalcogenides (TMDs) are commonly classified as quasi-two-dimensional materials, meaning that their electronic structure closely resembles that of an individual layer, which results in resistivity anisotropies reaching thousands. Here, we show that this rule does not hold for 1T-TaS2 - a compound with the richest phase diagram among TMDs. While the onset of charge density wave order makes the in-plane conduction non-metallic, we reveal that the out-of-plane charge transport is metallic and the resistivity anisotropy is close to one. We support our findings with ab-initio calculations predicting a pronounced quasi-one-dimensional character of the electronic structure. Consequently, we interpret the highly debated metal-insulator transition in 1T-TaS2 as a quasi-one-dimensional instability, contrary to the long-standing Mott localisation picture. In a broader context, these findings are relevant for the newly born field of van der Waals heterostructures, where tuning interlayer interactions (e.g. by twist, strain, intercalation, etc.) leads to new emergent phenomena., Comment: 41 page including supplementary information, 5 main figures, 13 supplementary figures. To be published in npj 2D Materials and Applications

We employ angle resolved photoemission spectroscopy (ARPES) to investigate the Fermi surface of RuO$_2$. We find a network of two Dirac nodal lines (DNL) as previously predicted in theory, where the valence- and conduction bands touch along continuous lines in momentum space. In addition, we find evidence for a third DNL close to the Fermi level which appears robust despite the presence of significant spin orbit coupling. We demonstrate that the third DNL gives rise to a topologically trivial flat-band surface state (FBSS) at the (110) surface. This FBSS can be tuned by surface doping and presents an interesting playground for the study of surface chemistry and exotic correlation phenomena., Comment: 12 pages, 9 figures

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 Cu3Bi(SeO3)2O2Cl 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 hightemperatures, 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 softmode 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 behaviour 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., Comment: 6 pages, 5 Figures, supplemental material included

Through a combined theoretical and experimental effort, we uncover a yet unidentified mechanism that strengthens considerably electron-phonon coupling in materials where electron accumulation leads to population of multiple valleys. Taking atomically-thin transition-metal dichalcogenides as prototypical examples, we establish that the mechanism results from a phonon-induced out-of-phase energy shift of the different valleys, which causes inter-valley charge transfer and reduces the effectiveness of electrostatic screening, thus enhancing electron-phonon interactions. The effect is physically robust, it can play a role in many materials and phenomena, as we illustrate by discussing experimental evidence for its relevance in the occurrence of superconductivity. (short abstract due to size limitations - full abstract in the manuscript), Comment: 16 pages, 8 figures

Time reversal and spatial inversion are two key symmetries for conventional Bardeen-Cooper-Schrieffer (BCS) superconductivity. Breaking inversion symmetry can lead to mixed-parity Cooper pairing and unconventional superconducting properties. Two-dimensional (2D) NbSe$_2$ has emerged as a new non-centrosymmetric superconductor with the unique out-of-plane or Ising spin-orbit coupling (SOC). Here, we report the observation of an unusual continuous paramagnetic-limited superconductor-normal metal transition in 2D NbSe$_2$. Using tunneling 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 superconductors. 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 NbSe$_2$. Our findings establish 2D NbSe$_2$ as a promising platform for exploring novel spin-dependent superconducting phenomena and device concepts, such as equal-spin Andreev reflection and topological superconductivity.

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., Comment: Nano Letters 2018

The semimetal MoTe$_2$ is studied by spin- and angle- resolved photoemission spectroscopy to probe the detailed electronic structure underlying its broad range of response behavior. A novel spin-texture is uncovered in the bulk Fermi surface of the non-centrosymmetric structural phase that is consistent with first-principles calculations. The spin-texture is three-dimensional, both in terms of momentum dependence and spin-orientation, and is not completely suppressed above the centrosymmetry-breaking transition temperature. Two types of surface Fermi arc are found to persist well above the transition temperature. The appearance of a large Fermi arc depends strongly on thermal history, and the electron quasiparticle lifetimes are greatly enhanced in the initial cooling. The results indicate that polar instability with strong electron-lattice interactions exists near the surface when the bulk is largely in a centrosymmetric phase.

The ability to gate-induce superconductivity by electrostatic charge accumulation is a recent breakthrough in physics and nano-electronics. With the exception of LaAlO$_3$/SrTiO$_3$ interfaces, experiments on gate-induced superconductors have been largely confined to resistance measurements, which provide very limited information about the superconducting state. Here, we explore gate-induced superconductivity in MoS$_2$ by performing tunneling spectroscopy to determine the energy-dependent density of states (DOS) for different levels of electron density $\textit{n}$. In the superconducting state, the DOS is strongly suppressed at energy smaller than the gap, \Delta, which is maximum (\Delta ~ 2 meV) for $\textit{n}$ of ~ 10$^{14}$ cm$^{-2}$ and decreases monotonously for larger $\textit{n}$. A perpendicular magnetic field $\textit{B}$ generates states at $E<\Delta$ that fill the gap, but a 20% DOS suppression of superconducting origin unexpectedly persists much above the transport critical field. Conversely, an in-plane field up to 10 T leaves the DOS entirely unchanged. Our measurements exclude that the superconducting state in MoS$_2$ is fully gapped and reveal the presence of a DOS that vanishes linearly with energy, the explanation of which requires going beyond a conventional, purely phonon-driven Bardeen-Cooper-Schrieffer mechanism.

We present a state-of-the-art density functional theory (DFT) study which models crucial features of the partially disordered orbital order stacking in the prototypical layered transition metal dichalcogenide 1T-TaS2 . Our results not only show that DFT models with realistic assumptions about the orbital order perpendicular to the layers yield band structures which agree remarkably well with experiments. They also demonstrate that DFT correctly predicts the formation of an excitation pseudo-gap which is commonly attributed to Mott-Hubbard type electron-electron correlations. These results highlight the importance of interlayer interactions in layered transition metal dichalcogenides and serve as an intriguing example of how disorder within an electronic crystal can give rise to pseudo-gap features.

We report on the magnetocrystalline anisotropy energy (MAE) and spin reorientation in antiferromagnetic state of spin $S=1/2$ tetramer system SeCuO$_3$ observed in torque magnetometry measurements in magnetic fields $H<5$~T and simulated using density functional calculations. We employ simple phenomenological model of spin reorientation in finite magnetic field to describe our experimental torque data. Our results strongly support collinear model for magnetic structure in zero field with possibility of only very weak canting. Torque measurements also indicate that, contrary to what is expected for uniaxial antiferromagnet, in SeCuO$_3$ only part of the spins exhibit spin flop instead all of them, allowing us to conclude that AFM state of SeCuO$_3$ is unconventional and comprised of two decoupled subsystems. Taking into account previously proposed site-selective correlations and dimer singlet state formation in this system, our results offer further proof that AFM state in SeCuO$_3$ is composed of a subsystem of AFM dimers forming singlets immersed in antiferromagnetically long-range ordered spins, where both states coexist on atomic scale. Furthermore, we show, using an ab-initio approach, that both subsystems contribute differently to the MAE, corroborating the existence of decoupled subnetworks in SeCuO$_3$. Combination of torque magnetometry, phenomenological approach and DFT simulations to magnetic anisotropy presented here represents a unique and original way to study site-specific reorientation phenomena in quantum magnets., Comment: 15 pages, 12 figures, submitted

It is well known that superconductivity in thin films is generally suppressed with decreasing thickness. This suppression is normally governed by either disorder-induced localization of Cooper pairs, weakening of Coulomb screening, or generation and unbinding of vortex-antivortex pairs as described by the Berezinskii-Kosterlitz-Thouless (BKT) theory. Defying general expectations, few-layer NbSe2 - an archetypal example of ultrathin superconductors - has been found to remain superconducting down to monolayer thickness. Here we report measurements of both the superconducting energy gap and critical temperature in high-quality monocrystals of few-layer NbSe2, using planar-junction tunneling spectroscopy and lateral transport. We observe a fully developed gap that rapidly reduces for devices with the number of layers N < 5, as does their ctitical temperature. We show that the observed reduction cannot be explained by disorder, and the BKT mechanism is also excluded by measuring its transition temperature that for all N remains very close to Tc. We attribute the observed behavior to changes in the electronic band structure predicted for mono- and bi- layer NbSe2 combined with inevitable suppression of the Cooper pair density at the superconductor-vacuum interface. Our experimental results for N > 2 are in good agreement with the dependences of the gap and Tc expected in the latter case while the effect of band-structure reconstruction is evidenced by a stronger suppression of the gap and the disappearance of its anisotropy for N = 2. The spatial scale involved in the surface suppression of the density of states is only a few angstroms but cannot be ignored for atomically thin superconductors., Comment: 21 pages, including supporting information

We present an experimental investigation of the magnetic structure in a tetramer system SeCuO$_3$ using neutron diffraction and nuclear resonance techniques. We establish a non-collinear, commensurate antiferromagnetic ordering with a propagation vector $\textbf{k} = \left(0,0,1 \right)$. The order parameter follows a critical behavior near $T_N = 8$ K, with a critical exponent $\beta = 0.32$ in agreement with a 3D universality class. Evidence is presented that a singlet state starts to form on tetramers at temperatures as high as 200 K, and its signature is preserved within the ordered state through a strong renormalization of the ordered magnetic moment on two non-equivalent copper sites, $m_{Cu1} \approx 0.4 \mu_B$ and $m_{Cu2} \approx 0.7 \mu_B$ at 1.5 K.

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 non-equilibrium 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 photo-generated neutral excitons and charged trions, and not by inter-band 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 photo-induced 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., Comment: accepted for publication in Nano Letters

The controversy regarding the precise nature of the high-temperature phase of 1T-TiSe2 lasts for decades. It has intensified in recent times when new evidence for the excitonic origin of the low-temperature charge-density wave state started to unveil. Here we address the problem of the high-temperature phase through precise measurements and detailed analysis of the optical response of 1T-TiSe2 single crystals. The separate responses of electron and hole subsystems are identified and followed in temperature. We show that neither semiconductor nor semimetal pictures can be applied in their generic forms as the scattering for both types of carriers is in the vicinity of the Ioffe-Regel limit with decay rates being comparable to or larger than the offsets of band extrema. The nonmetallic temperature dependence of transport properties comes from the anomalous temperature dependence of scattering rates. Near the transition temperature the heavy electrons and the light holes contribute equally to the conductivity. This surprising coincidence is regarded as the consequence of dominant intervalley scattering that precedes the transition. The low-frequency peak in the optical spectra is identified and attributed to the critical softening of the L-point collective mode., Comment: 28 pages, 10 figures

We present results from light scattering experiments on three insulating antiferromagnetic cuprates, YBa$_2$Cu$_3$O$_{6.05}$, Bi$_2$Sr$_2$YCu$_2$O$_{8+\delta}$, and La$_2$CuO$_4$ as a function of polarization and excitation energy {using samples of the latest generation. From the raw data we derive symmetry-resolved spectra.} The spectral shape in $B_{1g}$ symmetry is found to be nearly universal and independent of the excitation energy. The spectra agree quantitatively with predictions by field theory [\onlinecite{Weidinger:2015}] facilitating the precise extraction of the Heisenberg coupling $J$. {In addition, the asymmetric line shape on the high-energy side is found to be related to amplitude fluctuations of the magnetization. In La$_2$CuO$_4$ alone minor contributions from resonance effects may be identified.} The spectra in the other symmetries are not universal. The variations may be traced back to weak resonance effects and extrinsic contributions. For all three compounds we find support for the existence of chiral excitations appearing as a continuum in $A_{2g}$ symmetry having an onset slightly below $3J$. In La$_2$CuO$_4$ an additional isolated excitation appears on top of the $A_{2g}$ continuum., Comment: 8 pages, 7 figures

High-resolution angle-resolved photoemission spectroscopy (ARPES) data reveal evidence of a crossover from one-dimensional (1D) to three-dimensional (3D) behavior in the prototypical charge density wave (CDW) material NbSe3. In the low-temperature 3D regime, gaps in the electronic structure are observed due to two incommensurate CDWs, in agreement with x-ray diffraction and electronic-structure calculations. At higher temperatures we observe a spectral weight depletion that approaches the power-law behavior expected in 1D. From the warping of the quasi-1D Fermi surface at low temperatures, we extract the energy scale of the dimensional crossover. This is corroborated by a detailed analysis of the density of states, which reveals a change in dimensional behavior dependent on binding energy. Our results offer an important insight into the dimensionality of excitations in quasi-1D materials., Comment: Main text: 5 pages, 4 figures; Supplemental Material: 5 pages, 8 figures

We use a combination of experimental techniques to demonstrate a general occurrence of spin-orbit interaction (SOI) in graphene on transition metal dichalcogenide (TMD) substrates. Our measurements indicate that SOI is ultra-strong and extremely robust, despite it being merely interfacially-induced, with neither graphene nor the TMD substrates changing their structure. This is found to be the case irrespective of the TMD material used, of the transport regime, of the carrier type in the graphene band, and of the thickness of the graphene multilayer. Specifically, we perform weak antilocalization measurements as the simplest and most general diagnostic of SOI, and show that the spin relaxation time is very short in all cases regardless of the elastic scattering time. Such a short spin-relaxation time strongly suggests that the SOI originates from a modification of graphene band structure. We confirmed this expectation by measuring a gate-dependent beating, and a corresponding frequency splitting, in the low-field Shubnikov-de Haas magneto-resistance oscillations in high quality bilayer graphene on WSe$_2$. These measurements provide an unambiguous diagnostic of a SOI-induced splitting in the electronic band structure, and their analysis allows us to determine the SOI coupling constants for the Rashba term and the so-called spin-valley coupling term, i.e., the terms that were recently predicted theoretically for interface-induced SOI in graphene. The magnitude of the SOI splitting is found to be on the order of 10 meV, more than 100 times greater than the SOI intrinsic to graphene. Both the band character of the interfacially induced SOI, as well as its robustness and large magnitude make graphene-on-TMD a promising system to realize and explore a variety of spin-dependent transport phenomena, such as, in particular, spin-Hall and valley-Hall topological insulating states., Comment: 14 pages, 8 figures

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, accompanied by a correlated evolution of the CDW order. We find that the doping dependence of the superconducting and CDW phase transition in 2D NbSe$_2$ can be understood by a varying electron-phonon coupling strength induced by the gate-modulated carrier density and the electronic density of states near the Fermi surface.

We examine the experimental and theoretical electron-energy loss spectra in 2$H$-Cu$_{0.2}$NbS$_2$ and find that the 1 eV plasmon in this material does not exhibit the regular positive quadratic plasmon dispersion that would be expected for a normal broad-parabolic-band system. Instead we find a nearly non-dispersing plasmon in the momentum-transfer range $q<0.35$ \AA$^{-1}$. We argue that for a stoichiometric pure 2$H$-NbS$_2$ the dispersion relation is expected to have a negative slope as is the case for other transition-metal dichalcogenides. The presence of Cu impurities, required to stabilize the crystal growth, tends to shift the negative plasmon dispersion into a positive one, but the doping level in the current system is small enough to result in a nearly-non-dispersing plasmon. We conclude that a negative-slope plasmon dispersion is not connected with the existence of a charge-density-wave order in transition metal dichalcogenides.

Recently, the switching between the different charge-ordered phases of 1T-TaS2 has been probed by ultrafast techniques, revealing unexpected phenomena such as "hidden" metastable states and peculiar photoexcited charge patterns. Here, we apply broadband pump-probe spectroscopy with varying excitation energy to study the ultrafast optical properties of 1T-TaS2 in the visible regime. By scanning the excitation energy in the near-IR region we unravel the coupling between different charge excitations and the low-lying charge-density wave state. We find that the amplitude mode of the charge-density wave exhibits strong coupling to a long-lived doublon state that is photoinduced in the center of the star-shaped charge-ordered Ta clusters by the near-IR optical excitation.