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Magnetic fields can have profound effects on the motion of electrons in quantum materials. Two-dimensional (2D) electron systems subject to strong magnetic fields are expected to exhibit quantized Hall conductivity, chiral edge currents, and distinctive collective modes referred to as magnetoplasmons and magnetoexcitons. Generating these propagating collective modes in charge-neutral samples and imaging them at their native nanometer length scales have thus far been experimentally elusive tasks. In this study, we visualize propagating magenetoexction polaritons at their native length scales and report their magnetic-field-tunable dispersions in near-charge-neutral graphene. Imaging of these collective modes and their associated opto-electrical responses at the sample edges is enabled by innovations to our cryogenic near-field optical microscope that allows us to nano-image the optical responses of 2D materials in magnetic fields up to 7 Tesla. This novel nano-magneto-optics approach represents a new paradigm for exploring and manipulating magnetopolaritons in specimens with low carrier doping via harnessing high magnetic fields.

Metals are canonical plasmonic media at infrared and optical wavelengths, allowing one to guide and manipulate light at the nanoscale. A special form of optical waveguiding is afforded by highly anisotropic crystals revealing the opposite signs of the dielectric functions along orthogonal directions. These media are classified as hyperbolic and include crystalline insulators, semiconductors, and artificial metamaterials. Layered anisotropic metals are also anticipated to support hyperbolic waveguiding. However, this behavior remains elusive, primarily because interband losses arrest the propagation of infrared modes. Here, we report on the observation of propagating hyperbolic waves in a prototypical layered nodal-line semimetal ZrSiSe. The observed waveguiding originates from polaritonic hybridization between near-infrared light and nodal-line plasmons. Unique nodal electronic structures simultaneously suppress interband loss and boost the plasmonic response, ultimately enabling the propagation of infrared modes through the bulk of the crystal.

Van-der Waals (vdW) atomically layered crystals can act as optical waveguides over a broad range of the electromagnetic spectrum ranging from Terahertz to visible. Unlike common Si-based waveguides, vdW semiconductors host strong excitonic resonances that may be controlled using non-thermal stimuli including electrostatic gating and photoexcitation. Here, we utilize waveguide modes to examine photo-induced changes of excitons in the prototypical vdW semiconductor, WSe2, prompted by femtosecond light pulses. Using time-resolved scanning near-field optical microscopy we visualize the electric field profiles of waveguide modes in real space and time and extract the temporal evolution of the optical constants following femtosecond photoexcitation. By monitoring the phase velocity of the waveguide modes, we detect incoherent A-exciton bleaching along with a coherent optical Stark shift in WSe2. The authors use time-resolved scanning near-field optical microscopy to probe the ultrafast excitonic processes and their impact on waveguide operation in transition metal dichalcogenide crystals. They observe significant modulation of the complex index by monitoring waveguide modes on the fs time scale, and identify both coherent and incoherent manipulations of WSe2 excitonic resonances.

Metals are canonical plasmonic media at infrared and optical wavelengths allowing one to guide and manipulate light at sub-diffractional length scales. A special form of optical waveguiding is offered by highly anisotropic crystals revealing different signs of the dielectric function along orthogonal directions. These latter types of media are classified as hyperbolic and many crystalline insulators, semiconductors and artificial metal-based metamaterials belong to that class. Layered anisotropic metals are also anticipated to support hyperbolic waveguiding. Yet this behavior remains elusive primarily because interband processes introduce extreme losses and arrest light propagation. Here, we report on the observation of propagating hyperbolic waves in a prototypical layered nodal-line semimetal ZrSiSe. The unique electronic structure with touching energy bands at nodal points/lines suppresses losses and enables a hyperbolic regime at the telecommunications frequencies. The observed waveguiding in metallic ZrSiSe is a product of polaritonic hybridization between near-infrared light and long-lived nodal-line plasmons. By mapping the energy-momentum dispersion of the nodal-line hyperbolic modes in ZrSiSe we inquired into the role of additional screening associated with the surface states.

Chiral Weyl fermions with linear energy-momentum dispersion in the bulk accompanied by Fermi-arc states on the surfaces prompt a host of enticing optical effects. While new Weyl semimetal materials keep emerging, the available optical probes are limited. In particular, isolating bulk and surface electrodynamics in Weyl conductors remains a challenge. We devised an approach to the problem based on near-field photocurrent imaging at the nanoscale and applied this technique to a prototypical Weyl semimetal TaIrTe(4). As a first step, we visualized nano-photocurrent patterns in real space and demonstrated their connection to bulk nonlinear conductivity tensors through extensive modeling augmented with density functional theory calculations. Notably, our nanoscale probe gives access to not only the in-plane but also the out-of-plane electric fields so that it is feasible to interrogate all allowed nonlinear tensors including those that remained dormant in conventional far-field optics. Surface- and bulk-related nonlinear contributions are distinguished through their “symmetry fingerprints” in the photocurrent maps. Robust photocurrents also appear at mirror-symmetry breaking edges of TaIrTe(4) single crystals that we assign to nonlinear conductivity tensors forbidden in the bulk. Nano-photocurrent spectroscopy at the boundary reveals a strong resonance structure absent in the interior of the sample, providing evidence for elusive surface states.

Twisted two-dimensional van der Waals (vdW) heterostructures have unlocked a new means for manipulating the properties of quantum materials. The resulting mesoscopic moiré superlattices are accessible to a wide variety of scanning probes. To date, spatially-resolved techniques have prioritized electronic structure visualization, with lattice response experiments only in their infancy. Here, we therefore investigate lattice dynamics in twisted layers of hexagonal boron nitride (hBN), formed by a minute twist angle between two hBN monolayers assembled on a graphite substrate. Nano-infrared (nano-IR) spectroscopy reveals systematic variations of the in-plane optical phonon frequencies amongst the triangular domains and domain walls in the hBN moiré superlattices. Our first-principles calculations unveil a local and stacking-dependent interaction with the underlying graphite, prompting symmetry-breaking between the otherwise identical neighboring moiré domains of twisted hBN., Here, the authors investigate the lattice dynamics of twisted hexagonal boron nitride layers via nano-infrared spectroscopy, showing local and stacking-dependent variations of the optical phonon frequencies associated to the interaction with the graphite substrate.

Tungsten ditelluride (WTe2) is an atomically layered transition metal dichalcogenide whose physical properties change systematically from monolayer to bilayer and few-layer versions. In this report, we use apertureless scattering-type near-field optical microscopy operating at Terahertz (THz) frequencies and cryogenic temperatures to study the distinct THz range electromagnetic responses of mono-, bi- and trilayer WTe2 in the same multi-terraced micro-crystal. THz nano-images of monolayer terraces uncovered weakly insulating behavior that is consistent with transport measurements. The near-field signal on bilayer regions shows moderate metallicity with negligible temperature dependence. Subdiffractional THz imaging data together with theoretical calculations involving thermally activated carriers favor the semimetal scenario with $$\Delta \approx -10\,{{{\rm{meV}}}}$$ Δ ≈ − 10 meV over the semiconductor scenario for bilayer WTe2. Also, we observed clear metallic behavior of the near-field signal on trilayer regions. Our data are consistent with the existence of surface plasmon polaritons in the THz range confined to trilayer terraces in our specimens. Finally, data for microcrystals up to 12 layers thick reveal how the response of a few-layer WTe2 asymptotically approaches the bulk limit.

Excitons play a dominant role in the optoelectronic properties of atomically thin van der Waals (vdW) semiconductors. These excitons are amenable to on-demand engineering with diverse control knobs, including dielectric screening, interlayer hybridization, and moiré potentials. However, external stimuli frequently yield heterogeneous excitonic responses at the nano- and meso-scales, making their spatial characterization with conventional diffraction-limited optics a formidable task. Here, we use a scattering-type scanning near-field optical microscope (s-SNOM) to acquire exciton spectra in atomically thin transition metal dichalcogenide microcrystals with previously unattainable 20 nm resolution. Our nano-optical data revealed material- and stacking-dependent exciton spectra of MoSe2, WSe2, and their heterostructures. Furthermore, we extracted the complex dielectric function of these prototypical vdW semiconductors. s-SNOM hyperspectral images uncovered how the dielectric screening modifies excitons at length scales as short as few nanometers. This work paves the way towards understanding and manipulation of excitons in atomically thin layers at the nanoscale., Excitons play an important role in the optical properties of 2D semiconductors, but their spatial characterization is usually constrained by the diffraction limit. Here, the authors report near-field optical spectroscopy of 2D transition metal dichalcogenides with 20 nm resolution, revealing their spatially dependent excitonic spectra and complex dielectric function.

Dirac fermions with highly dispersive linear bands1–3 are usually considered weakly correlated due to the relatively large bandwidths (W) compared to Coulomb interactions (U). With the discovery of nodal-line semimetals, the notion of the Dirac point has been extended to lines and loops in momentum space. The anisotropy associated with nodal-line structure gives rise to greatly reduced kinetic energy along the line. However, experimental evidence for the anticipated enhanced correlations in nodal-line semimetals is sparse. Here, we report on prominent correlation effects in a nodal-line semimetal compound, ZrSiSe, through a combination of optical spectroscopy and density functional theory calculations. We observed two fundamental spectroscopic hallmarks of electronic correlations: strong reduction (1/3) of the free-carrier Drude weight and also the Fermi velocity compared to predictions of density functional band theory. The renormalization of Fermi velocity can be further controlled with an external magnetic field. ZrSiSe therefore offers the rare opportunity to investigate correlation-driven physics in a Dirac system. What happens to topological materials when their electrons are strongly interacting is an open question. Shao and others demonstrate that ZrSiSe is a material that can address this as it has a topological band structure and non-trivial correlations.

Lighting a route for hyperbolic dispersion The propagation of light within a material is usually well defined, with the propagation described by scattering and dispersion. In artificially designed metamaterials and in anisotropic layered materials, the dispersion can be hyperbolic, giving rise to subwavelength confinement of the light. Sternbach et al. show that the hyperbolic dispersion can be optically switched on and off on demand in the layered transition metal dichalcogenide tungsten diselenide (see the Perspective by Deng and Chen). Illuminating the material with ultrafast pulses of sub-bandgap light creates a transient waveguide, resulting in hyperbolic dispersion in the material. The ability to tune the dispersion characteristics on demand using optical pumping is an effective approach for developing ultrafast switching photonic devices and controlling the propagation of light on the nanoscale. Science , this issue p. 617 ; see also p. 572

Tungsten ditelluride (WTe_2) is a transition metal dichalcogenide whose physical properties depend critically on the number of layers. In this paper, we use apertureless scattering-type near-field optical microscopy operating at Terahertz (THz) frequencies and cryogenic temperatures to identify distinct THz range electromagnetic behavior of WTe_2 mono-, bi- and tri-layer terraces in the same micro-crystals. We observed clear metallic behavior of the near-field signal on tri-layer regions. Our data are consistent with the existence of surface plasmon polaritons (SPP) in the THz range confined to tri-layer terraces in our specimens. The near-field signal on bi-layer regions surprisingly shows moderately metallicity, but with negligible temperature dependence. Subdiffractional THz imaging data together with theoretical calculations considering thermally activated carriers favor the semimetal scenario over the semiconductor scenario for bi-layer WTe_2. THz images for monolayer terraces uncovered weakly insulating behavior consistent with transport data.

Tungsten ditelluride (WTe2) is an atomically layered transition metal dichalcogenide whose physical properties change systematically from monolayer to bilayer and few-layer versions. In this report, we use apertureless scattering-type near-field optical microscopy operating at Terahertz (THz) frequencies and cryogenic temperatures to study the distinct THz range electromagnetic responses of mono-, bi- and trilayer WTe2 in the same multi-terraced micro-crystal. THz nano-images of monolayer terraces uncovered weakly insulating behavior that is consistent with transport measurements. The near-field signal on bilayer regions shows moderate metallicity with negligible temperature dependence. Subdiffractional THz imaging data together with theoretical calculations involving thermally activated carriers favor the semimetal scenario with \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$\Delta \approx -10\,{{{\rm{meV}}}}$$\end{document}Δ≈−10meV over the semiconductor scenario for bilayer WTe2. Also, we observed clear metallic behavior of the near-field signal on trilayer regions. Our data are consistent with the existence of surface plasmon polaritons in the THz range confined to trilayer terraces in our specimens. Finally, data for microcrystals up to 12 layers thick reveal how the response of a few-layer WTe2 asymptotically approaches the bulk limit., The behaviour of Tungsten ditelluride (WTe2) in few-layer form is not yet fully characterized. Here the authors use a near-field terahertz microscopy technique to observe the electromagnetic responses of WTe2 flakes from one to several layers and to study their semimetallic/ semiconducting behavior.

The osmate pyrochlore Cd2Os2O7 supports an antiferromagnet insulator ground state with an all-in/all-out (AIAO) spin ordering at low temperature. Above 225 K, Cd2Os2O7 becomes a paramagnetic metal whereas the mechanism of this metal-to-insulator transition (MIT) remains elusive. In this letter, we use cryogenic near-field technique operating at terahertz frequencies to study the evolution of low-energy response across the MIT. We observed a systematic variation of the magnitude of nano-THz signal across the transition, consistent with the trend in the direct-current conductivity. Conducting domain walls that dominate the nano-scale landscape of the conductivity of a closely related AIAO system Nd2Ir2O7 are not apparent in Cd2Os2O7.

Significance The 3D nodal points in Dirac and/or Weyl semimetals are in the vanguard of quantum materials research. A hallmark of these systems is the linear band dispersion. This latter electronic stricture gives rise to unconventional transport and optical phenomena. Here, we demonstrate that solids with dispersive nodal lines in the electronic structure share many common aspects with the response of 3D nodal-points systems. We investigated N b A s 2 using a combination of optical and magneto-optical techniques and have identified electromagnetic signature of dispersive nodal lines. This particular compound has allowed us to inquire the impact of spin-orbit coupling on the universal characteristic of nodal metals.

Photonic crystals are commonly implemented in media with periodically varying optical properties. Photonic crystals enable exquisite control of light propagation in integrated optical circuits, and also emulate advanced physical concepts. However, common photonic crystals are unfit for in-operando on/off controls. We overcome this limitation and demonstrate a broadly tunable two-dimensional photonic crystal for surface plasmon polaritons. Our platform consists of a continuous graphene monolayer integrated in a back-gated platform with nano-structured gate insulators. Infrared nano-imaging reveals the formation of a photonic bandgap and strong modulation of the local plasmonic density of states that can be turned on/off or gradually tuned by the applied gate voltage. We also implement an artificial domain wall which supports highly confined one-dimensional plasmonic modes. Our electrostatically-tunable photonic crystals are derived from standard metal oxide semiconductor field effect transistor technology and pave a way for practical on-chip light manipulation., Traditional photonic crystals consist of periodic media with a pre-defined optical response. Here, the authors combine nanostructured back-gate insulators with a continuous layer of graphene to demonstrate an electrically tunable two-dimensional photonic crystal suitable for controlling the propagation of surface plasmon polaritons.

Using magneto-infrared spectroscopy, we have explored the charge dynamics of (Bi,Sb)$_2$Te$_3$ thin films on InP substrates. From the magneto-transmission data we extracted three distinct cyclotron resonance (CR) energies that are all apparent in the broad band Faraday rotation (FR) spectra. This comprehensive FR-CR data set has allowed us to isolate the response of the bulk states from the intrinsic surface states associated with both the top and bottom surfaces of the film. The FR data uncovered that electron- and hole-type Dirac fermions reside on opposite surfaces of our films, which paves the way for observing many exotic quantum phenomena in topological insulators., 5 pages, accepted by Nano Lett (2016)

We report mid-infrared spectroscopy measurements of ultrathin, electrostatically gated (Bi_(1-x)Sb_x)_2Te_3 topological insulator films, in which we observe several percent modulation of transmittance and reflectance as gating shifts the Fermi level. Infrared transmittance measurements of gated films were enabled by use of an epitaxial lift-off method for large-area transfer of topological insulator films from infrared-absorbing SrTiO3 growth substrates to thermal oxidized silicon substrates. We combine these optical experiments with transport measurements and angle-resolved photoemission spectroscopy to identify the observed spectral modulation as a gate-driven transfer of spectral weight between both bulk and 2D topological surface channels and interband and intraband channels. We develop a model for the complex permittivity of gated (Bi_(1-x)Sb_x)_2Te_3, and find a good match to our experimental data. These results open the path for layered topological insulator materials as a new candidate for tunable, ultrathin infrared optics and highlight the possibility of switching topological optoelectronic phenomena between bulk and spin-polarized surface regimes.

Knowing the band structure of materials is one of the prerequisites to understand their properties. Therefore, especially in the last decades, angle-resolved photoemission spectroscopy (ARPES) has become a highly demanded experimental tool to investigate the band structure. However, especially in thin film materials with a layered structure and several capping layers, access to the electronic structure by ARPES is limited. Therefore, several alternative methods to obtain the required information have been suggested. Here, we directly invert the results by cyclotron resonance experiments to obtain the band structure of a two-dimensional (2D) material. This procedure is applied to the mercury telluride quantum well with critical thickness which is characterized by a 2D electron gas with linear dispersion relations. The Dirac-like band structure in this material could be mapped both on the electron and on the hole side of the band diagram. In this material, purely linear dispersion of the hole-like carriers is in contrast to detectable quadratic corrections for the electrons., 18 pages, 6 figures

We investigated emission and propagation of polaritons in a two dimensional van der Waals material hexagonal boron nitride (hBN). Our specific emphasis in this work is on hyperbolic phonon polariton emission that we investigated by means of scattering-type scanning near-field optical microscopy. Real-space nano-images detail how the polaritons are launched in several common arrangements including: light scattering by the edges of the crystal, metallic nanostructures deposited on the surface of hBN crystals, as well as random defects and impurities. Notably, the scanned tip of the near-field microscope is itself an efficient polariton launcher. Our analysis reveals that the scanning tips are superior to other types of emitters we have investigated. Furthermore, the study of polariton emission and emission efficiency may provide insights for development of polaritonic devices and for fundamental studies of collective modes in other van der Waals materials.

We investigated the $ab$-plane optical properties of single crystals of ${\mathrm{WTe}}_{2}$ for light polarized parallel and perpendicular to the W-chain axis over a broad range of frequency and temperature. At far-infrared frequencies, we observed a striking dependence of the reflectance edge on light polarization, corresponding to anisotropy of the carrier effective masses. We quantitatively studied the temperature dependence of the plasma frequency, revealing a modest increase of the effective mass anisotropy in the $ab$ plane upon cooling. We also found strongly anisotropic interband transitions persisting to high photon energies. These results were analyzed by comparison with ab initio calculations. The calculated and measured plasma frequencies agree to within 10% for both polarizations, while the calculated interband conductivity shows excellent agreement with experiment.

We report mid-infrared spectroscopy measurements of ultrathin, electrostatically gated (Bi

We report measurements of London penetration depth $\lambda(T)$ for the noncentrosymmetric superconductor BiPd by using a tunnel diode oscillator. Pronounced anisotropic behavior is observed in the low-temperature penetration depth; the in-plane penetration depth $\lambda_{ac}(T)$ follows an exponential decrease, but the interplane penetration depth $\lambda_b(T)$ shows power-law-type behavior. The superfluid density $\rho_s(T)$, converted from the penetration depth $\lambda(T)$, is best fitted by an anisotropic two-band BCS model. We argue that such a complex order parameter is attributed to the admixture of spin-singlet and spin-triplet pairing states as a result of antisymmetric spin-orbit coupling in BiPd., Comment: 5 pages, 4 figure, to be published in Phys. Rev. B (Rapid Communication)