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We present CoTe2 as a new type-II Dirac semimetal supporting Lorentz symmetry violating Dirac fermions in the vicinity of the Fermi energy. By combining first principle ab-initio calculations with experimental angle-resolved photo-emission spectroscopy results, we show the CoTe2 hosts a pair of type-II Dirac fermions around 90 meV above the Fermi energy. In addition to the bulk Dirac fermions, we find several topological band inversions in bulk CoTe2, which gives rise to a ladder of spin-polarized surface states over a wide range of energies. In contrast to the surface states which typically display Rashba-type in-plane spin splitting, we find that CoTe2 hosts novel out-of-plane spin polarization as well. Our work establishes CoTe2 as a potential candidate for the exploration of Dirac fermiology and applications in spintronic devices, infrared plasmonics, and ultrafast optoelectronics., Comment: 9 pages,7 figures, Accepted in Phys. Rev. B

Magnetic materials exhibiting topological Dirac fermions are attracting significant attention for their promising technological potential in spintronics. In these systems, the combined effect of the spin-orbit coupling and magnetic order enables the realization of novel topological phases with exotic transport properties, including the anomalous Hall effect and magneto-chiral phenomena. Herein, we report experimental signature of topological Dirac antiferromagnetism in TaCoTe2 via angle-resolved photoelectron spectroscopy (ARPES) and first-principles density functional theory (DFT) calculations. In particular, we find the existence of spin-orbit coupling-induced gaps at the Fermi level, consistent with the manifestation of a large intrinsic non-linear Hall conductivity. Remarkably, we find that the latter is extremely sensitive to the orientation of the N\'eel vector, suggesting TaCoTe2 a suitable candidate for the realization of non-volatile spintronic devices with an unprecedented level of intrinsic tunability.

Plasmonics in topological semimetals offers exciting opportunities for fundamental physics exploration as well as for technological applications. Here, we investigate plasmons in the exemplar chiral crystal CoSi, which hosts a variety of multifold fermionic excitations. We show that CoSi hosts two distinct plasmon modes in the infrared regime at 0.1 eV and 1.1 eV in the long-wavelength limit. The 0.1 eV plasmon is found to be highly dispersive, and originates from intraband collective oscillations associated with a double spin-1 excitation, while the 1.1 eV plasmon is dispersionless and it involves interband correlations. Both plasmon modes lie outside the particle-hole continuum and possess long lifetime. Our study indicates that the CoSi class of materials will provide an interesting materials platform for exploring fundamental and technological aspects of topological plasmonics.

Compared to artificial metamaterials, where nano-fabrication complexities and finite-size inclusions can hamper the desired electromagnetic response, several natural materials like van der Waals crystals hold great promise for designing efficient nanophotonic devices in the optical range. Here, we investigate the unusual optical response of NiTe$_2$, a van der Waals crystal and a type-II Dirac semimetal hosting Lorentz-violating Dirac fermions. By {\it ab~initio~} density functional theory modeling, we show that NiTe$_2$ harbors multiple topological photonic regimes for evanescent waves (such as surface plasmons) across the near-infrared and optical range. By electron energy-loss experiments, we identify surface plasmon resonances near the photonic topological transition points at the epsilon-near-zero (ENZ) frequencies $\approx 0.79$, $1.64$, and $2.22$ eV. Driven by the extreme crystal anisotropy and the presence of Lorentz-violating Dirac fermions, the experimental evidence of ENZ surface plasmon resonances confirm the non-trivial photonic and electronic topology of NiTe$_2$. Our study paves the way for realizing devices for light manipulation at the deep-subwavelength scales based on electronic and photonic topological physics for nanophotonics, optoelectronics, imaging, and biosensing applications., Comment: 12 pages, 11 figures

The ZrSiS family of compounds hosts various exotic quantum phenomena due to the presence of both topological nonsymmorphic Dirac fermions and nodal-line fermions. In this material family, the LnSbTe (Ln= lanthanide) compounds are particularly interesting owing to the intrinsic magnetism from magnetic Ln which leads to new properties and quantum states. In this work, the authors focus on the previously unexplored compound SmSbTe. The studies reveal a rare combination of a few functional properties in this material, including antiferromagnetism with possible magnetic frustration, electron correlation enhancement, and Dirac nodal-line fermions. These properties enable SmSbTe as a unique platform to explore exotic quantum phenomena and advanced functionalities arising from the interplay between magnetism, topology, and electronic correlations., Comment: 23 pages, 5 figures

Using spin- and angle- resolved photoemission spectroscopy (spin-ARPES) together with ${\it ab~initio}$ calculations, we demonstrate the existence of a type-II Dirac semimetal state in NiTe$_2$. We show that, unlike PtTe$_2$, PtSe$_2$, and PdTe$_2$, the Dirac node in NiTe$_2$ is located in close vicinity of the Fermi energy. Additionally, NiTe$_2$ also hosts a pair of band inversions below the Fermi level along the $\Gamma-A$ high-symmetry direction, with one of them leading to a Dirac cone in the surface states. The bulk Dirac nodes and the ladder of band inversions in NiTe$_2$ support unique topological surface states with chiral spin texture over a wide range of energies. Our work paves the way for the exploitation of the low-energy type-II Dirac fermions in NiTe$_2$ in the fields of spintronics, THz plasmonics and ultrafast optoelectronics., Comment: 4+ pages and 4 figures; minor revision

We predict the existence of a novel long-lived gapless plasmon mode in a type-II Dirac semimetal (DSM). This gapless mode arises from the out-of-phase oscillations of the density fluctuations in the electron and the hole pockets of a type-II DSM. It originates beyond a critical wave-vector along the direction of the tilt axis, owing to the momentum separation of the electron and hole pockets. A similar out-of-phase plasmon mode arises in other multi-component charged fluids as well, but generally it is Landau damped and lies within the particle-hole continuum. In the case of a type-II DSM, the open Fermi surface prohibits low-energy finite momentum single-particle excitations, creating a `gap' in the particle-hole continuum. The gapless plasmon mode lies within this particle-hole continuum gap and, thus, it is protected from Landau damping., Comment: 5 pages, 3 figurers. Comments are welcome

Topological insulators are innovative materials with semiconducting bulk together with surface states forming a Dirac cone, which ensure metallic conduction in the surface plane. Therefore, topological insulators represent an ideal platform for optoelectronics and photonics. The recent progress of science and technology based on topological insulators enables the exploitation of their huge application capabilities. Here, we review the recent achievements of optoelectronics, photonics and plasmonics with topological insulators. Plasmonic devices and photodetectors based on topological insulators in a wide energy range, from Terahertz to the ultraviolet, promise outstanding impact. Furthermore, the peculiarities, the range of applications and the challenges of the emerging fields of topological photonics and thermoplasmonics are discussed.

Single- and few-layered InSe flakes are produced by the liquid-phase exfoliation of beta-InSe single crystals in 2-propanol, obtaining stable dispersions with a concentration as high as 0.11 g/L. Ultracentrifugation is used to tune the morphology, i.e., the lateral size and thickness of the as-produced InSe flakes. We demonstrate that the obtained InSe flakes have maximum lateral sizes ranging from 30 nm to a few um, and thicknesses ranging from 1 to 20 nm, with a max population centred at ~ 5 nm, corresponding to 4 Se-In-In-Se quaternary layers. We also show that no formation of further InSe-based compounds (such as In2Se3) or oxides occurs during the exfoliation process. The potential of these exfoliated-InSe few-layer flakes as a catalyst for hydrogen evolution reaction (HER) is tested in hybrid single-walled carbon nanotubes/InSe heterostructures. We highlight the dependence of the InSe flakes morphologies, i.e., surface area and thickness, on the HER performances achieving best efficiencies with small flakes offering predominant edge effects. Our theoretical model unveils the origin of the catalytic efficiency of InSe flakes, and correlates the catalytic activity to the Se vacancies at the edge of the flakes., Comment: 39 pages

The discovery of graphene triggered a rapid rise of unexplored two-dimensional materials and heterostructures having optoelectronic and photonics properties that can be tailored on the nanoscale. Among these materials, black phosphorus (BP) has attracted a remarkable interest thanks to many favorable properties, such as high carrier mobility, in-plane anisotropy, the possibility to alter its transport via electrical gating and direct band-gap, that can be tuned by thickness from 0.3 eV (bulk crystalline) to 1.7 eV (single atomic layer). When integrated in a microscopic field effect transistor (FET), a few-layer BP flake can detect Terahertz (THz) frequency radiation. Remarkably, the in-plane crystalline anisotropy can be exploited to tailor the mechanisms that dominate the photoresponse; a BP-based field effect transistor can be engineered to act as a plasma-wave rectifier, a thermoelectric sensor or a thermal bolometer. Here we present a review on recent research on BP detectors operating from 0.26 THz to 3.4 THz with particular emphasis on the underlying physical mechanisms and the future challenges that are yet to be addressed for making BP the active core of stable and reliable optical and electronic technologies.

Near-field imaging with terahertz (THz) waves is emerging as a powerful technique for fundamental research in photonics and across physical and life sciences. Spatial resolution beyond the diffraction limit can be achieved by collecting THz waves from an object through a small aperture placed in the near-field. However, light transmission through a sub-wavelength size aperture is fundamentally limited by the wave nature of light. Here, we conceive a novel architecture that exploits inherently strong evanescent THz field arising within the aperture to mitigate the problem of vanishing transmission. The sub-wavelength aperture is originally coupled to asymmetric electrodes, which activate the thermo-electric THz detection mechanism in a transistor channel made of flakes of black-phosphorus or InAs nanowires. The proposed novel THz near-field probes enable room-temperature sub-wavelength resolution coherent imaging with a 3.4 THz quantum cascade laser, paving the way to compact and versatile THz imaging systems and promising to bridge the gap in spatial resolution from the nanoscale to the diffraction limit.

Chemical doping of bulk black phosphorus is a well-recognized way to reduce surface oxidation and degradation. Here, we report on the fabrication of terahertz frequency detectors consisting of an antenna-coupled field-effect transistor (FET) with an active channel of Se-doped black phosphorus. Our devices show a maximum room-temperature hole mobility of 1780 cm2V-1s-1 in a SiO2-encapsulated FET. A room-temperature responsivity of 3 V/W was observed, with a noise-equivalent power of 7 nWHz-1/2 at 3.4 THz, comparable with the state-of-the-art room-temperature photodetectors operating at the same frequency. Therefore, the inclusion of Se dopants in the growth process of black phosphorus crystals enables the optimization of the transport and optical performances of FETs in the far-infrared with a high potential for the development of BP-based electro-optical devices. We also demonstrate that the flake thickness can be tuned according to the target application. Specifically, thicker flakes (>80 nm) are suitable for applications in which high mobility and high speed are essential, thinner flakes (<10 nm) are more appropriate for applications requiring high on/off ratios, while THz photodetection is optimal with flakes 30-40 nm thick, due to the larger carrier density tunability., Comment: 8 pages, 4 figures. This is the pre-peer reviewed, authors' version of the Nanoscale article, published in its final form at doi: 10.1039/c8nr09060b

By means of high-resolution electron energy loss spectroscopy, we investigate the low-energy excitation spectrum of transition-metal monopnictides hosting Weyl fermions. We observe gapped plasmonic modes in (001)-oriented surfaces of single crystals of NbAs and TaAs at 66 and 68 meV, respectively. Our findings are consistent with theory and we estimate an effective Coulomb interaction strength $\alpha_{\rm eff}\approx0.41$ for both samples. We also demonstrate that the modification of the surface of transition-metal monopnictides by the adsorption of chemical species (in our case, oxygen and hydrocarbon fragments) changes the frequency of the plasmonic excitations, with a subsequent modification of the effective interaction strength in the 0.30-0.48 range. The remarkable dependence of plasmonic features on the presence of adsorbates paves the way for plasmonic sensors based on Weyl semimetals operating in the mid-infrared., Comment: 7 pages, 3 figures

We explore the broadband excitation spectrum of bulk PtTe$_2$ using electron energy loss spectroscopy and density functional theory. In addition to infrared modes related to intraband 3D Dirac plasmon and interband transitions between the 3D Dirac bands, we observe modes at 3.9, 7.5 and 19.0 eV in the ultraviolet region. The comparison of the excitation spectrum with the calculated orbital-resolved density of states allows us to ascribe spectral features to transitions between specific electronic states. Additionally, we study the thickness dependence of the high-energy plasmon in the PtTe2 thin films. We show that, unlike graphene, the high-energy plasmon in PtTe2 thin film gets red-shifted by 2.5 eV with increasing thickness., Comment: 9 pages with 7 figures

In this minireview, we explore the main features and the prospect of plasmonics with two-dimensional semiconductors. Plasmonic modes in each class of van der Waals semiconductors have their own peculiarities, along with potential technological capabilities. Plasmons of transition-metal dichalcogenides share features typical of graphene, due to their honeycomb structure, but with damping processes dominated by intraband rather than interband transitions, unlike graphene. Spin-orbit coupling strongly affects the plasmonic spectrum of buckled honeycomb lattices (silicene and germanene), while the anisotropic lattice of phosphorene determines different propagation of plasmons along the armchair and zigzag direction. We also review existing applications of plasmonics with two-dimensional materials in the fields of thermoplasmonics, biosensing, and plasma-wave Terahertz detection. Finally, we consider the capabilities of van der Waals heterostructures for innovative low-loss plasmonic devices., Comment: 8 pages, 4 figures, This is the pre-peer reviewed, authors' version of the published Nanoscale article, 2018; minor revision

Artificial semiconductor heterostructures played a pivotal role in modern electronic and photonic technologies, providing a highly effective mean for the manipulation and control of carriers, from the visible to the Terahertz (THz) frequency range. Despite the exceptional versatility, they commonly require challenging epitaxial growth procedures due to the need of clean and abrupt interfaces, which proved to be a major obstacle for the realization of room-temperature (RT), high-efficiency devices, like source, detectors or modulators, especially in the far-infrared. Two-dimensional (2D) layered materials, like graphene and phosphorene, recently emerged as a reliable, flexible and versatile alternative for devising efficient RT detectors operating at Terahertz frequencies. We here combine the benefit of the heterostructure architecture with the exceptional technological potential of 2D layered nanomaterials; by reassembling the thin isolated atomic planes of hexagonal borum nitride (hBN) with a few layer phosphorene (black phosphorus (BP)) we mechanically stacked hBN/BP/hBN heterostructures to devise high-efficiency THz photodetectors operating in the 0.3-0.65 THz range from 4K to 300K with a record SNR=20000.

The discovery of graphene and the related fascinating capabilities have triggered an unprecedented interest in inorganic two-dimensional (2D) materials. Despite the impressive impact in a variety of photonic applications, the absence of energy gap has hampered its broader applicability in many optoelectronic devices. The recent advance of novel 2D materials, such as transition-metal dichalcogenides or atomically thin elemental materials, (e.g. silicene, germanene and phosphorene) promises a revolutionary step-change. Here we devise the first room-temperature Terahertz (THz) frequency detector exploiting few-layer phosphorene, e.g., a 10 nm thick flake of exfoliated crystalline black phosphorus (BP), as active channel of a field-effect transistor (FET). By exploiting the direct band gap of BP to fully switch between insulating and conducting states and by engineering proper antennas for efficient light harvesting, we reach detection performance comparable with commercial detection technologies, providing the first technological demonstration of a phosphorus-based active THz device.

Topological insulators (TIs) represent a novel quantum state of matter, characterized by edge or surface-states, showing up on the topological character of the bulk wave functions. Allowing electrons to move along their surface, but not through their inside, they emerged as an intriguing material platform for the exploration of exotic physical phenomena, somehow resembling the graphene Dirac-cone physics, as well as for exciting applications in optoelectronics, spintronics, nanoscience, low-power electronics, and quantum computing. Investigation of topological surface states (TSS) is conventionally hindered by the fact that in most of experimental conditions the TSS properties are mixed up with those of bulk-states. Here, we devise a novel tool to unveil TSS and to probe related plasmonic effects. By engineering Bi2Te(3-x)Sex stoichiometry, and by gating the surface of nanoscale field-effect-transistors, exploiting thin flakes of Bi2Te2.2Se0.8 or Bi2Se3, we provide the first demonstration of room-temperature Terahertz (THz) detection mediated by over-damped plasma-wave oscillations on the "activated" TSS of a Bi2Te2.2Se0.8 flake. The reported detection performances allow a realistic exploitation of TSS for large-area, fast imaging, promising superb impacts on THz photonics.

By means of vibrational spectroscopy and density functional theory (DFT), we investigate CO adsorption on phosphorene-based systems. We find stable CO adsorption at room temperature on both phosphorene and bulk black phosphorus. The adsorption energy and vibrational spectrum have been calculated for several possible configurations of the CO overlayer. We find that the vibrational spectrum is characterized by two different C-O stretching energies. The experimental data are in good agreement with the prediction of the DFT model and unveil the unusual C-O vibrational band at 165-180 meV, activated by the lateral interactions in the CO overlayer.

We have studied the electronic excitation spectrum in periodically rippled graphene on Ru(0001) and flat, commensurate graphene on Ni(111) by means of high-resolution electron energy loss spectroscopy and a combination of density functional theory and tight-binding approaches. We show that the periodic moir\'e superlattice originated by the lattice mismatch in graphene/Ru(0001) induces the emergence of an extra mode, which is not present in graphene/Ni(111). Contrary to the ordinary intra-band plasmon of doped graphene, the extra mode is robust in charge-neutral graphene/metal contacts, having its origin in electron-hole inter-band transitions between van Hove singularities that emerge in the reconstructed band structure, due to the moir\'e pattern superlattice., Comment: Supplemental materials available at http://www.theorphys.science.ru.nl/people/yuan/

The interaction of graphene with metallic substrates reveals phenomena and properties of great relevance for applications in nanotechnology. In this review, the vibrational characterization by means of various inelastic scattering spectroscopies are surveyed for graphene epitaxially grown on metals and transition carbides. In particular, the manifestations of electron-phonon interaction, such as Kohn anomalies, the evaluation of elastic properties and the nanoscale control of phonon modes are presented and discussed., Comment: in press, (25 figures, review paper). Critical Reviews in Solid State and Materials Sciences, 2016

In neutral graphene, two prominent cusps known as Kohn anomalies are found in the phonon dispersion of the highest optical phonon at $q=\Gamma$ (LO branch) and $q=K$ (TO branch), reflecting a significant electron-phonon coupling to undoped Dirac electrons. In this work, high-resolution electron energy loss spectroscopy is used to measure the phonon dispersion around the $\Gamma$ point in quasi-freestanding graphene epitaxially grown on Pt(111). The Kohn anomaly for the LO phonon is observed at finite momentum $q\sim2k_F$ from $\Gamma$, with a shape in excellent agreement with the theory and consistent with known values of the EPC and the Fermi level. More strikingly, we also observe a Kohn anomaly at the same momentum for the out-of-plane optical phonon (ZO) branch. This observation is the first direct evidence of the coupling of the ZO mode with Dirac electrons, which is forbidden for freestanding graphene but becomes allowed in the presence of a substrate. Moreover, we estimate the EPC to be even greater than that of the LO mode, making graphene on Pt(111) an optimal system to explore the effects of this new coupling in the electronic properties., Comment: Final version with journal reference. Significantly more experimental data was added to the main text and the supplemental material. 5 pages of main text + 6 of supplement

When the phonon spectrum of a material is measured in a scattering experiment, selection rules preclude the observation of phonons that are odd under reflection by the scattering plane. Understanding these rules is crucial to correctly interpret experiments and to detect broken symmetries. Taking graphene as a case study, in this work we derive the complete set of selection rules for the honeycomb lattice, showing that some of them have been missed or misinterpreted in the literature. Focusing on the technique of high-resolution electron energy loss spectroscopy (HREELS), we calculate the scattering intensity for a simple force constant model to illustrate these rules. In addition, we present HREELS measurements of the phonon dispersion for graphene on Ru(0001) and find excellent agreement with the theory. We also illustrate the effect of different symmetry breaking scenarios in the selection rules and discuss previous experiments in light of our results., Comment: 8 pages, 5 figures

Graphene epitaxially grown on Ru(0001) displays a remarkably ordered pattern of hills and valleys in Scanning Tunneling Microscopy (STM) images. To which extent the observed "ripples" are structural or electronic in origin have been much disputed recently. A combination of ultrahigh resolution STM images and Helium Atom diffraction data shows that i) the graphene lattice is rotated with respect to the lattice of Ru and ii) the structural corrugation as determined from He diffraction is substantially smaller (0.015 nm) than predicted (0.15 nm) or reported from X-Ray Diffraction or Low Energy Electron Diffraction. The electronic corrugation, on the contrary, is strong enough to invert the contrast between hills and valleys above +2.6 V as new, spatially localized electronic states enter the energy window of the STM. The large electronic corrugation results in a nanostructured periodic landscape of electron and holes pockets., Comment: 16 pages, 6 figures