Highly confined epsilon-near-zero and surface phonon polaritons in SrTiO3 membranes.

Recent theoretical studies have suggested that transition metal perovskite oxide membranes can enable surface phonon polaritons in the infrared range with low loss and much stronger subwavelength confinement than bulk crystals. Such modes, however, have not been experimentally observed so far. Here, using a combination of far-field Fourier-transform infrared (FTIR) spectroscopy and near-field synchrotron infrared nanospectroscopy (SINS) imaging, we study the phonon polaritons in a 100 nm thick freestanding crystalline membrane of SrTiO3 transferred on metallic and dielectric substrates. We observe a symmetric-antisymmetric mode splitting giving rise to epsilon-near-zero and Berreman modes as well as highly confined (by a factor of 10) propagating phonon polaritons, both of which result from the deep-subwavelength thickness of the membranes. Theoretical modeling based on the analytical finite-dipole model and numerical finite-difference methods fully corroborate the experimental results. Our work reveals the potential of oxide membranes as a promising platform for infrared photonics and polaritonics.

Thermal and electrostatic tuning of surface phonon-polaritons in LaAlO3/SrTiO3 heterostructures.

Phonon polaritons are promising for infrared applications due to a strong light-matter coupling and subwavelength energy confinement they offer. Yet, the spectral narrowness of the phonon bands and difficulty to tune the phonon polariton properties hinder further progress in this field. SrTiO3 - a prototype perovskite oxide - has recently attracted attention due to two prominent far-infrared phonon polaritons bands, albeit without any tuning reported so far. Here we show, using cryogenic infrared near-field microscopy, that long-propagating surface phonon polaritons are present both in bare SrTiO3 and in LaAlO3/SrTiO3 heterostructures hosting a two-dimensional electron gas. The presence of the two-dimensional electron gas increases dramatically the thermal variation of the upper limit of the surface phonon polariton band due to temperature dependent polaronic screening of the surface charge carriers. Furthermore, we demonstrate a tunability of the upper surface phonon polariton frequency in LaAlO3/SrTiO3 via electrostatic gating. Our results suggest that oxide interfaces are a new platform bridging unconventional electronics and long-wavelength nanophotonics.

Infrared nano-imaging of Dirac magnetoexcitons in graphene.

Magnetic fields can have profound effects on the motion of electrons in quantum materials. Two-dimensional 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 nanometre length scales have thus far been experimentally elusive. Here we visualize propagating magnetoexciton polaritons at their native length scales and report their magnetic-field-tunable dispersion in near-charge-neutral graphene. Imaging these collective modes and their associated nano-electro-optical responses allows us to identify polariton-modulated optical and photo-thermal electric effects at the sample edges, which are the most pronounced near charge neutrality. Our work is enabled by innovations in cryogenic near-field optical microscopy techniques that allow for the nano-imaging of the near-field responses of two-dimensional materials under magnetic fields up to 7 T. This nano-magneto-optics approach allows us to explore and manipulate magnetopolaritons in specimens with low carrier doping via harnessing high magnetic fields.

Controlling Magnetism with Light in a Zero Orbital Angular Momentum Antiferromagnet.

Antiferromagnetic materials feature intrinsic ultrafast spin dynamics, making them ideal candidates for future magnonic devices operating at THz frequencies. A major focus of current research is the investigation of optical methods for the efficient generation of coherent magnons in antiferromagnetic insulators. In magnetic lattices endowed with orbital angular momentum, spin-orbit coupling enables spin dynamics through the resonant excitation of low-energy electric dipoles such as phonons and orbital resonances which interact with spins. However, in magnetic systems with zero orbital angular momentum, microscopic pathways for the resonant and low-energy optical excitation of coherent spin dynamics are lacking. Here, we consider experimentally the relative merits of electronic and vibrational excitations for the optical control of zero orbital angular momentum magnets, focusing on a limit case: the antiferromagnet manganese phosphorous trisulfide (MnPS_{3}), constituted by orbital singlet Mn^{2+} ions. We study the correlation of spins with two types of excitations within its band gap: a bound electron orbital excitation from the singlet orbital ground state of Mn^{2+} into an orbital triplet state, which causes coherent spin precession, and a vibrational excitation of the crystal field that causes thermal spin disorder. Our findings cast orbital transitions as key targets for magnetic control in insulators constituted by magnetic centers of zero orbital angular momentum.

Nanoinfrared Characterization of Bilayer Graphene Conductivity under Dual-Gate Tuning.

Dual-gate tuning on two-dimensional (2D) heterostructures can provide independent control of the carrier concentration and interlayer electrostatic potential, yielding novel electronic and optical properties. In this paper, by utilizing monolayer graphene as both the top gate and a plasmon wavelength magnifier, the optical properties of bilayer graphene (BLG) under dual-gate are quantitatively investigated by nanoinfrared imaging. The hybrid optical modes in the vertically coupled two-layer system are imaged from scattering-type scanning near-field microscopy (s-SNOM). Moreover, plasmon dispersion behaviors under varied dual-gate tuning are explored and explained well with theoretical ones employing tight binding approximation, which reveals the flexibility in individually manipulating the Fermi energy and bandgap. Especially, electron-hole asymmetry in BLG is verified from experiments. Our studies pave route for quantitative near-field investigation of superlattice, topological boundaries, and other emergent phenomena in graphene-based 2D heterostructures.

Colossal infrared and terahertz magneto-optical activity in a two-dimensional Dirac material.

When two-dimensional electron gases (2DEGs) are exposed to a magnetic field, they resonantly absorb electromagnetic radiation via electronic transitions between Landau levels1. In 2DEGs with a Dirac spectrum, such as graphene, theory predicts an exceptionally high infrared magneto-absorption, even at zero doping2-5. However, the measured Landau-level magneto-optical effects in graphene have been much weaker than expected2,6-12 because of imperfections in the samples available for such experiments. Here, we measure magneto-transmission and Faraday rotation in high-mobility encapsulated monolayer graphene using a custom-designed set-up for magneto-infrared microspectroscopy. Our results show strongly enhanced magneto-optical activity in the infrared and terahertz ranges, characterized by absorption of light near to the 50% maximum allowed, 100% magnetic circular dichroism and high Faraday rotation. Considering that sizeable effects have been already observed at routinely achievable magnetic fields, our findings demonstrate the potential of magnetic tuning in 2D Dirac materials for long-wavelength optoelectronics and plasmonics.

High sensitivity variable-temperature infrared nanoscopy of conducting oxide interfaces.

Probing the local transport properties of two-dimensional electron systems (2DES) confined at buried interfaces requires a non-invasive technique with a high spatial resolution operating in a broad temperature range. In this paper, we investigate the scattering-type scanning near field optical microscopy as a tool for studying the conducting LaAlO3/SrTiO3 interface from room temperature down to 6 K. We show that the near-field optical signal, in particular its phase component, is highly sensitive to the transport properties of the electron system present at the interface. Our modeling reveals that such sensitivity originates from the interaction of the AFM tip with coupled plasmon-phonon modes with a small penetration depth. The model allows us to quantitatively correlate changes in the optical signal with the variation of the 2DES transport properties induced by cooling and by electrostatic gating. To probe the spatial resolution of the technique, we image conducting nano-channels written in insulating heterostructures with a voltage-biased tip of an atomic force microscope.

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

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

Electrically controlled terahertz magneto-optical phenomena in continuous and patterned graphene.

The magnetic circular dichroism and the Faraday rotation are the fundamental phenomena of great practical importance arising from the breaking of the time reversal symmetry by a magnetic field. In most materials, the strength and the sign of these effects can be only controlled by the field value and its orientation. Furthermore, the terahertz range is lacking materials having the ability to affect the polarization state of the light in a non-reciprocal manner. Here we demonstrate, using broadband terahertz magneto-electro-optical spectroscopy, that in graphene both the magnetic circular dichroism and the Faraday rotation can be modulated in intensity, tuned in frequency and, importantly, inverted using only electrostatic doping at a fixed magnetic field. In addition, we observe strong magneto-plasmonic resonances in a patterned array of graphene antidots, which potentially allows exploiting these magneto-optical phenomena in a broad THz range.

Suppressed Magnetic Circular Dichroism and Valley-Selective Magnetoabsorption due to the Effective Mass Anisotropy in Bismuth.

We measure the far-infrared reflectivity and Kerr angle spectra on a high-quality crystal of pure semimetallic bismuth as a function of magnetic field, from which we extract the conductivity for left- and right-handed circular polarizations. The high spectral resolution allows us to separate the intraband Landau level transitions for electrons and holes. The hole transition exhibits 100% magnetic circular dichroism; it appears only for one polarization as expected for a circular cyclotron orbit. However, the dichroism for electron transitions is reduced to only 13±1%, which is quantitatively explained by the large effective mass anisotropy of the electron pockets of the Fermi surface. This observation is a signature of the mismatch between the metric experienced by the photons and the electrons. It allows for a contactless measurement of the effective mass anisotropy and provides a direction towards valley polarized magnetooptical pumping with elliptically polarized light.

Near optimal graphene terahertz non-reciprocal isolator.

Isolators, or optical diodes, are devices enabling unidirectional light propagation by using non-reciprocal optical materials, namely materials able to break Lorentz reciprocity. The realization of isolators at terahertz frequencies is a very important open challenge made difficult by the intrinsically lossy propagation of terahertz radiation in current non-reciprocal materials. Here we report the design, fabrication and measurement of a terahertz non-reciprocal isolator for circularly polarized waves based on magnetostatically biased monolayer graphene, operating in reflection. The device exploits the non-reciprocal optical conductivity of graphene and, in spite of its simple design, it exhibits almost 20 dB of isolation and only 7.5 dB of insertion loss at 2.9 THz. Operation with linearly polarized light can be achieved using quarter-wave plates as polarization converters. These results demonstrate the superiority of graphene with respect to currently used terahertz non-reciprocal materials and pave the way to a novel class of optimal non-reciprocal devices.

Versatile setup for optical spectroscopy under high pressure and low temperature.

We present an optical setup for spectroscopic measurements in the infrared and of Raman shift under high pressure and at low temperature. Using a membrane-driven diamond anvil cell, the pressure can be tuned in situ up to 20 GPa and the temperatures ranges from room temperature down to 18 K in transmission mode and 13 K in reflection mode. In transmission, the setup is entirely working under vacuum to reduce the water absorption features and obtain a higher spectral stability. Since the infrared throughput obtained with a thermal source is limited, the use of a synchrotron source allowed to enhance the performance, as illustrated with results obtained with various materials. The analysis of the reflectivity is adapted so that it benefits from ambient pressure data and produces quantitative optical conductivity curves that can be easily compared to the results at ambient pressure.

Magneto-optical Kramers-Kronig analysis.

We describe a simple magneto-optical experiment and introduce a magneto-optical Kramers-Kronig analysis (MOKKA) that together allow extracting the complex dielectric function for left- and right-handed circular polarizations in a broad range of frequencies without actually generating circularly polarized light. The experiment consists of measuring reflectivity and Kerr rotation, or alternatively transmission and Faraday rotation, at normal incidence using only standard broadband polarizers without retarders or quarter-wave plates. In a common case, where the magneto-optical rotation is small (below ∼0.2 rad), a fast measurement protocol can be realized, where the polarizers are fixed at 45(∘) with respect to each other. Apart from the time-effectiveness, the advantage of this protocol is that it can be implemented at ultra-high magnetic fields and in other situations, where an in-situ polarizer rotation is difficult. Overall, the proposed technique can be regarded as a magneto-optical generalization of the conventional Kramers-Kronig analysis of reflectivity on bulk samples and the Kramers-Kronig constrained variational analysis of more complex types of spectral data. We demonstrate the application of this method to the textbook semimetals bismuth and graphite and also use it to obtain handedness-resolved magneto-absorption spectra of graphene on SiC.

Mono- and bilayer WS2 light-emitting transistors.

We have realized ambipolar ionic liquid gated field-effect transistors based on WS2 mono- and bilayers, and investigated their opto-electronic response. A thorough characterization of the transport properties demonstrates the high quality of these devices for both electron and hole accumulation, which enables the quantitative determination of the band gap (Δ1L = 2.14 eV for monolayers and Δ2L = 1.82 eV for bilayers). It also enables the operation of the transistors in the ambipolar injection regime with electrons and holes injected simultaneously at the two opposite contacts of the devices in which we observe light emission from the FET channel. A quantitative analysis of the spectral properties of the emitted light, together with a comparison with the band gap values obtained from transport, show the internal consistency of our results and allow a quantitative estimate of the excitonic binding energies to be made. Our results demonstrate the power of ionic liquid gating in combination with nanoelectronic systems, as well as the compatibility of this technique with optical measurements on semiconducting transition metal dichalcogenides. These findings further open the way to the investigation of the optical properties of these systems in a carrier density range much broader than that explored until now.

Strong plasmon reflection at nanometer-size gaps in monolayer graphene on SiC.

We employ tip-enhanced infrared near-field microscopy to study the plasmonic properties of epitaxial quasi-free-standing monolayer graphene on silicon carbide. The near-field images reveal propagating graphene plasmons, as well as a strong plasmon reflection at gaps in the graphene layer, which appear at the steps between the SiC terraces. When the step height is around 1.5 nm, which is two orders of magnitude smaller than the plasmon wavelength, the reflection signal reaches 20% of its value at graphene edges, and it approaches 50% for step heights as small as 5 nm. This intriguing observation is corroborated by numerical simulations and explained by the accumulation of a line charge at the graphene termination. The associated electromagnetic fields at the graphene termination decay within a few nanometers, thus preventing efficient plasmon transmission across nanoscale gaps. Our work suggests that plasmon propagation in graphene-based circuits can be tailored using extremely compact nanostructures, such as ultranarrow gaps. It also demonstrates that tip-enhanced near-field microscopy is a powerful contactless tool to examine nanoscale defects in graphene.

Fabry-Perot enhanced Faraday rotation in graphene.

We demonstrate that giant Faraday rotation in graphene in the terahertz range due to the cyclotron resonance is further increased by constructive Fabry-Perot interference in the supporting substrate. Simultaneously, an enhanced total transmission is achieved, making this effect doubly advantageous for graphene-based magneto-optical applications. As an example, we present far-infrared spectra of epitaxial multilayer graphene grown on the C-face of 6H-SiC, where the interference fringes are spectrally resolved and a Faraday rotation up to 0.15 radians (9°) is attained. Further, we discuss and compare other ways to increase the Faraday rotation using the principle of an optical cavity.

Surface state charge dynamics of a high-mobility three-dimensional topological insulator.

We present a magneto-optical study of the three-dimensional topological insulator, strained HgTe, using a technique which capitalizes on advantages of time-domain spectroscopy to amplify the signal from the surface states. This measurement delivers valuable and precise information regarding the surface-state dispersion within <1 meV of the Fermi level. The technique is highly suitable for the pursuit of the topological magnetoelectric effect and axion electrodynamics.