Search

Phonon polaritons (PhPs) (light coupled to lattice vibrations) in the highly anisotropic polar layered material molybdenum trioxide (\alpha-MoO_3) are currently the focus of intense research efforts due to their extreme subwavelength field confinement, directional propagation and unprecedented low losses. Nevertheless, prior research has primarily concentrated on exploiting the squeezing and steering capabilities of \alpha-MoO_3 PhPs, without inquiring much into the dominant microscopic mechanism that determines their long lifetimes, key for their implementation in nanophotonic applications. This study delves into the fundamental processes that govern PhP damping in \alpha-MoO_3 by combining ab initio calculations with scattering-type scanning near-field optical microscopy (s-SNOM) and Fourier-transform infrared (FTIR) spectroscopy measurements across a broad temperature range (from 8 to 300 K). The remarkable agreement between our theoretical predictions and experimental observations allows us to identify third-order anharmonic phonon-phonon scattering as the main damping mechanism of \alpha-MoO_3 PhPs. These findings shed light on the fundamental limits of low-loss PhPs, a crucial factor for assessing their implementation into nanophotonic devices., Comment: 24 pages, 4 figures

Twisted bilayer graphene (TBG) represents a highly tunable, strongly correlated electron system owed to its unique flat electronic bands. However, understanding the single-particle band structure alone has been challenging due to complex lattice reconstruction effects and a lack of spectroscopic measurements over a broad energy range. Here, we probe the band structure of TBG around the magic angle using infrared spectroscopy. Our measurements reveal spectral features originating from interband transitions whose energies are uniquely defined by the twist angle. By combining with quantum transport, we connect spectral features over a broad energy range (10 to 700 meV) spanning several superlattice minibands and track their evolution with twist angle. We compare our data with calculations of the band structures obtained via the continuum model and find good agreement only when considering a variation of interlayer/intralayer tunnelling parameters with the twist angle. Our analysis suggests that the magic angle also shifts due to lattice relaxation, and is better defined for a wide angular range from 0.9{\deg} to 1.1{\deg}. Our work provides spectroscopic insights into TBG's band structure and offers an optical fingerprint of the magic angle for screening heterostructures before nanofabrication.

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.

In topological photonics, artificial photonic structures are constructed for realizing nontrivial unidirectional propagation of photonic information. On the other hand, moir\'e superlattices are emerging as an important avenue for engineering quantum materials with novel properties. In this paper, we combine these two aspects and demonstrate theoretically that moir\'e superlattices of small-angle twisted monolayer-bilayer graphene provide a natural platform for valley protected plasmons. Particularly, a complete plasmonic bandgap appears stemming from the distinct optical conductivities of the ABA and ABC stacked triangular domains. Moreover, the plasmonic crystals exhibit nonzero valley Chern numbers and unidirectional transport of plasmonic edge states protected from inter-valley scattering is presented.

Polaritons are light-matter quasiparticles that govern the optical response of quantum materials and enable their nanophotonic applications. We have studied a new type of polaritons arising in magnetized graphene encapsulated in hexagonal boron nitride (hBN). These polaritons stem from hybridization of Dirac magnetoexciton modes of graphene with waveguide phonon modes of hBN crystals. We refer to these quasiparticles as the Landau-phonon polaritons (LPPs). Using infrared magneto nanoscopy, we imaged LPPs and controlled their real-space propagation by varying the magnetic field. These LLPs have large in-plane momenta and are not bound by the conventional optical selection rules, granting us access to the "forbidden" inter-Landau level transitions (ILTs). We observed avoided crossings in the LPP dispersion - a hallmark of the strong coupling regime - occurring when the magnetoexciton and hBN phonon frequencies matched. Our LPP-based nanoscopy also enabled us to resolve two fundamental many-body effects: the graphene Fermi velocity renormalization and ILT-dependent magnetoexciton binding energies. These results indicate that magnetic-field-tuned Dirac heterostructures are promising platforms for precise nanoscale control and sensing of light-matter interaction.

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., Comment: Nature Communications, in press

Some correlated materials display an insulator-to-metal transition as the temperature is increased. In most cases this transition can also be induced electrically, resulting in volatile resistive switching due to the formation of a conducting filament. While this phenomenon has attracted much attention due to potential applications, many fundamental questions remain unaddressed. One of them is its characteristic lengths: what sets the size of these filaments, and how does this impact resistive switching properties. Here we use a combination of wide-field and scattering-type scanning near-field optical microscopies to characterize filament formation in NdNiO3 and SmNiO3 thin films. We find a clear trend: smaller filaments increase the current density, yielding sharper switching and a larger resistive drop. With the aid of numerical simulations, we discuss the parameters controlling the filament width and, hence, the switching properties.

Nanoscale channels realized at the conducting interface between LaAlO$_{3}$ and SrTiO$_{3}$ provide a perfect playground to explore the effect of dimensionality on the electronic properties of complex oxides. Here we compare the electric transport properties of devices realized using the AFM-writing technique and conventional photo-lithography. We find that the lateral size of the conducting paths has a strong effect on their transport behavior at low temperature. We observe a crossover from metallic to insulating regime occurring at about 50 K for channels narrower than 100 nm. The insulating upturn can be suppressed by the application of a positive backgate. We compare the behavior of nanometric constrictions in lithographically patterned channels with the result of model calculations and we conclude that the experimental observations are compatible with the physics of a quantum point contact., Comment: 9 pages, 6 figures

When two-dimensional electron gases (2DEGs) are exposed to magnetic field, they resonantly absorb electromagnetic radiation via electronic transitions between Landau levels (LLs). In 2DEGs with a Dirac spectrum, such as graphene, theory predicts an exceptionally high infrared magneto-absorption, even at zero doping. However, the measured LL magneto-optical effects in graphene have been much weaker than expected because of imperfections in the samples available so far for such experiments. Here we measure magneto-transmission and Faraday rotation in high-mobility encapsulated monolayer graphene using a custom designed setup for magneto-infrared microspectroscopy. Our results show a strongly enhanced magneto-optical activity in the infrared and terahertz ranges characterized by a maximum allowed (50%) absorption of light, a 100% magnetic circular dichroism as well as a record high Faraday rotation. Considering that sizeable effects have been already observed at routinely achievable magnetic fields, our findings demonstrate a new potential of magnetic tuning in 2D Dirac materials for long-wavelength optoelectronics and plasmonics., Comment: 14 pages, 4 figures

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 modelling 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., Comment: 19 pages, 5 figures

Faraday rotation is a fundamental property present in all non-reciprocal optical elements. In the THz range, graphene displays strong Faraday rotation; unfortunately, it is limited to frequencies below the cyclotron resonance. Here we show experimentally that in specifically design metasurfaces, magneto-plasmons can be used to circumvent this limitation. We find excellent agreement between theory and experiment and provide new physical insights and predictions on these phenomena. Finally, we demonstrate strong tuneability in these metasurfaces using electric and magnetic field biasing., Comment: 5 pages, 3 figures

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 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 polarisation 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., Comment: 7 pages, 3 figures, supplementary information included

Graphene is a mechanically robust 2D material promising for flexible optoelectronic applications. However, its electromagnetic properties under strain are experimentally poorly understood. Here we present the far-infrared transmission spectra of large-area chemical-vapor deposited monolayer graphene on a polyethylene terephthalate substrate subjected to uniaxial strain. The effective strain value is calibrated using the Raman spectroscopy and corrected for a relaxation of wrinkles and folds seen directly by atomic-force microscopy. We find that while the Drude weight and the Fermi level remain constant, the scattering rate increases by more than 10% per 1% of applied strain, showing a high level of reproducibility during strain cycling. As a result, the electronic mobility and optical absorption of graphene at terahertz and lower frequencies appear to also be sensitive to strain, which opens pathways to control these key parameters mechanically. We suggest that such a functionality can be potentially used in flexible optoelectronic and microelectromechanical systems based on graphene. By combining our findings with existing theoretical models, we discuss the possible mechanisms of strain-controlled Drude scattering., Comment: 12 pages, 9 figures + supplementary information

In systems having an anisotropic electronic structure, such as the layered materials graphite, graphene and cuprates, impulsive light excitation can coherently stimulate specific bosonic modes, with exotic consequences for the emergent electronic properties. Here we show that the population of E$_{2g}$ phonons in the multiband superconductor MgB$_2$ can be selectively enhanced by femtosecond laser pulses, leading to a transient control of the number of carriers in the {\sigma}-electronic subsystem. The nonequilibrium evolution of the material optical constants is followed in the spectral region sensitive to both the a- and c-axis plasma frequencies and modeled theoretically, revealing the details of the $\sigma$-$\pi$ interband scattering mechanism in MgB$_2$., Comment: 5 pages, 3 figures, 7 supplemental pages, 6 supplemental figures

We have measured 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 polarisations. 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 polarisation as expected for a circular cyclotron orbit. However the dichroism for electron transitions is reduced to only $13\pm 1$%, 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 polarised magneto-optical pumping with elliptically polarised light.

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 $\sim$ 0.2 rad), a fast measurement protocol can be realized, where the polarizers are fixed at 45$^\circ$ 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 \emph{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., Comment: 11 pages, 4 figurs

Semiconducting transition metal dichalcogenides (TMDs) have emerged as materials that can be used to realize two-dimensional (2D) crystals possessing rather unique transport and optical properties. Most research has so far focused on sulfur and selenium compounds, while tellurium-based materials attracted little attention so far. As a first step in the investigation of Te-based semiconducting TMDs in this context, we have studied MoTe$_2$ crystals with thicknesses above 4 nm, focusing on surface transport and a quantitative determination of the gap structure. Using ionic-liquid gated transistors, we show that ambipolar transport at the surface of the material is reproducibly achieved, with hole and electron mobility values between 10 and 30 cm$^2$/Vs at room temperature. The gap structure is determined through three different techniques: ionic-liquid gated transistors and scanning tunneling spectroscopy, that allow the measurement of the indirect gap ($E_{ind}$), and optical transmission spectroscopy on crystals of different thickness, that enables the determination of both the direct ($E_{dir}$) and the indirect gap. We find that at room temperature $E_{ind}$ = 0.88 eV and $E_{dir}$ = 1.02 eV. Our results suggest that thin MoTe$_2$ layers may exhibit a transition to a direct gap before mono-layer thickness. They should also drastically extend the range of direct gaps accessible in 2D semiconducting TMDs., Comment: 14 pages, 4 figures. To appear in 2D Materials

We perform scanning photocurrent microscopy on WS2 ionic liquid-gated field effect transistors exhibiting high-quality ambipolar transport. By properly biasing the gate electrode we can invert the sign of the photocurrent showing that the minority photocarriers are either electrons or holes. Both in the electron- and the hole-doping regimes the photocurrent decays exponentially as a function of the distance between the illumination spot and the nearest contact, in agreement with a two-terminal Schottky-barrier device model. This allows us to compare the value and the doping dependence of the diffusion length of the minority electrons and holes on a same sample. Interestingly, the diffusion length of the minority carriers is several times larger in the hole accumulation regime than in the electron accumulation regime, pointing out an electron-hole asymmetry in WS2.

We report the magnetic field-dependent far-infrared reflectivity of polycrystalline bismuth. We observe four distinct absorptions that we attribute to magnetoplasmon resonances, which are collective modes of an electron-hole liquid in magnetic field and become optical and acoustic resonances of the electron-hole system in the small-field limit. The acoustic mode is expected only when the masses of distinct components are very different, which is the case in bismuth. In a polycrystal, where the translational symmetry is broken, a big shift of spectral weight to acoustic plasmon is possible. This enables us to detect an associated plasma edge. Although the polycrystal sample has grains of randomly distributed orientations, our reflectivity results can be explained by invoking only two, clearly distinct, series of resonances. In the limit of zero field, the optical modes of these two series converge onto plasma frequencies measured in monocrystal along the main optical axes., Comment: Accepted in PRB

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 ({\Delta}1L = 2.14 eV for monolayers and {\Delta}2L = 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., Comment: 22 pages, 6 figures, Nano Letters (2014)

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 ultra-narrow gaps. It also demonstrates that tip-enhanced near-field microscopy is a powerful contactless tool to examine nanoscale defects in graphene., Comment: Nano Letters (2013); manuscript + supporting information

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{\deg}) is attained. Further, we discuss and compare other ways to increase the Faraday rotation using the principle of an optical cavity.

We measure the far-infrared magneto-optical Kerr rotation and reflectivity spectra in graphite and achieve a highly accurate unified microscopic description of all data in a broad range of magnetic fields by taking rigorously the c-axis band dispersion and the trigonal warping into account. We find that the second- and the forth-order cyclotron harmonics are optically almost as strong as the fundamental resonance even at high fields. They must play, therefore, a major role in magneto-optical and magneto-plasmonic applications based on Bernal stacked graphite and multilayer graphene., Comment: 4 pages, 3 figures + Supplemental Material

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., Comment: Published version, online Sept 23, 2011

Optical Faraday rotation is one of the most direct and practically important manifestations of magnetically broken time-reversal symmetry. The rotation angle is proportional to the distance traveled by the light, and up to now sizeable effects were observed only in macroscopically thick samples and in two-dimensional electron gases with effective thicknesses of several nanometers. Here we demonstrate that a single atomic layer of carbon - graphene - turns the polarization by several degrees in modest magnetic fields. The rotation is found to be strongly enhanced by resonances originating from the cyclotron effect in the classical regime and the inter-Landau-level transitions in the quantum regime. Combined with the possibility of ambipolar doping, this opens pathways to use graphene in fast tunable ultrathin infrared magneto-optical devices.