Nanoscale-confined Terahertz Polaritons in a van der Waals Crystal
Thales V. A. G. de Oliveira, Tobias Nörenberg, Gonzalo Álvarez-Pérez, Lukas Wehmeier, Javier Taboada-Gutiérrez, Maximilian Obst, Franz Hempel, Eduardo J. H. Lee… 展开作者
Thales V. A. G. de Oliveira, Tobias Nörenberg, Gonzalo Álvarez-Pérez, Lukas Wehmeier, Javier Taboada-Gutiérrez, Maximilian Obst, Franz Hempel, Eduardo J. H. Lee, John M. Klopf, Ion Errea, Alexey Y. Nikitin, Susanne C. Kehr, Pablo Alonso-Gonzaléz, Lukas M. Eng
Electromagnetic field confinement is crucial for nanophotonic technologies, since it allows for enhancing light-matter interactions, thus enabling light manipulation in deep sub-wavelength scales. In the terahertz (THz) spectral range, radiation confinement is conventionally achieved with specially designed metallic structures - such as antennas or nanoslits - with large footprints due to the rather long wavelengths of THz radiation. In this context, phonon polaritons - light coupled to lattice vibrations - in van der Waals (vdW) crystals have emerged as a promising solution for controlling light beyond the diffraction limit, as they feature extreme field confinements and low optical losses. However, experimental demonstration of nanoscale-confined phonon polaritons at THz frequencies has so far remained elusive. Here, we provide it by employing scattering-type scanning near-field optical microscopy (s-SNOM) combined with a free-electron laser (FEL) to reveal a range of low-loss polaritonic excitations at frequencies from 8 to 12 THz in the vdW semiconductor $α-MoO_3$. We visualize THz polaritons with i) in-plane hyperbolic dispersion, ii) extreme nanoscale field confinement (below $λ_o/75$) and iii) long polariton lifetimes, with a lower limit of > 2 ps.
Interactions of few-cycle terahertz pulses with the induced optical polarization in a quantum-well microcavity reveal that the lower and higher exciton-polariton modes together with the optically forbidden 2p-exciton state form a unique Λ-type three-level system. Pronounced nonlinearities are observed via time-resolved strong-terahertz and weak-optical excitation spectroscopy and explained with a fully microscopic theory. The results show that the terahertz pulses strongly couple the exciton-polariton states to the 2p-exciton state while no resonant transition between the two polariton levels …
We consider the nonlinear terahertz emission by the system of cavity polaritons in the regime of polariton lasing. To account for the quantum nature of terahertz-polariton coupling we use the Lindblad master equation approach and demonstrate that quantum microcavities reveal rich variety of the nonlinear phenomena in terahertz range, including bistability, short THz pulse generation and THz switching.
Electric dipole transitions between different cavity polariton branches or between dressed atomic states with the same excitation number are strictly forbidden in centro-symmetric systems. For doped quantum wells in semiconductor microcavities, the strong coupling between an intersubband transition in the conduction band and a cavity mode produces two branches of intersubband cavity polaritons, whose normal-mode energy splitting is tunable and can be in the terahertz region. Here, we show that, by using asymmetric quantum wells, it is possible to have allowed dipolar transitions between differ…
Coherent sub-THz phonons incident on a gold grating that is deposited on a dielectric substrate undergo diffraction and thereby induce an alteration of the surface plasmon-polariton resonance. This results in efficient high-frequency modulation (up to 110 GHz) of the structure's reflectivity for visible light in the vicinity of the plasmon-polariton resonance. High modulation efficiency is achieved by designing a periodic nanostructure which provides both plasmon-polariton and phonon resonances. Our theoretical analysis shows that the dynamical alteration of the plasmon-polariton resonance is …
Terahertz emission between exciton-polariton branches in semiconductor microcavities is expected to be strongly stimulated in the polariton laser regime, due to the high density of particles in the lower state (final state stimulation effect). However, non-radiative scattering processes depopulate the upper state and greatly hinder the efficiency of such terahertz sources. In this work, we suggest a new scheme using multiple microcavities and exploiting the transition between two interband polariton branches located below the exciton level. We compare the non-radiative processes loss rates in …
We use linear response theory in order to compute the light absorption spectrum, in the terahertz band, of a polariton system composed by excitons in a quantum dot very strongly coupled to the lowest photon mode of a thin micropillar. In a thermalized (Bose condensed) system at low temperatures, the spectral function shows a peak (GDR) associated to a 1s - 2p exciton transition, enhanced by polariton effects. On the other hand, in a non-equilibrium system absorption is peaked at low energies. Thus, a measurement of terahertz absorption could give an indication of the degree of thermalization i…
The large oscillator strength of excitons in transition metal dichalcogenide layers facilitates the formation of exciton-polariton resonances for monolayers and van-der-Waals heterostructures embedded in optical microcavities. Here, we show, that locally changing the number of layers in a WSe2/hBN/WSe2 van-der-Waals heterostructure embedded in a monolithic, high-quality-factor cavity gives rise to a local variation of the coupling strength. This effect yields a polaritonic stair case potential, which we demonstrate at room temperature. Our result paves the way towards engineering local polarit…
Two-dimensional van der Waals (vdW) crystals can sustain various types of polaritons with strong electromagnetic confinements, making them highly attractive for the nanoscale photonic and optoelectronic applications. While extensive experimental and numerical studies are devoted to the polaritons of the vdW crystals, analytical models are sparse. Particularly, applying such a model to describe the polariton behaviors visualized by state-of-art near-field optical microscopy requires further investigation. Herein, we develop an analytical waveguide model to describe the polariton propagations in…
Depending on the relative rates of coupling and dissipation, a light-matter coupled system is either in the weak- or strong-coupling regime. Here, we present a unique system where the coupling rate continuously increases with an externally applied magnetic field while the dissipation rate remains constant, allowing us to monitor a weak-to-strong coupling transition as a function of magnetic field. We observed a Rabi splitting of a terahertz magnon mode in yttrium orthoferrite above a threshold magnetic field of ~14 T. Based on a microscopic theoretical model, we show that with increasing magne…
The strong-coupling regime between an electronic transition and the photonic mode of a optical resonator manifests itself in the lifting of the degeneracy between the two modes and the creation of two polariton states with mixed optical and electronic character. This phenomenon has been studied in atoms, excitons in semiconductors and quantum electrodynamics circuits based on Josephson junctions. Recently, there is also strong interest to study similar effects using intersubband transitions in quantum wells in the terahertz, where the ultra strong coupling regime can be reached and new physica…
Semiconductor microcavities can exhibit various macroscopic quantum phenomena, including Bose-Einstein condensation of polaritons, Bardeen-Cooper-Schrieffer (BCS) states of polaritons, and photon lasing (lasing with negligible Coulombic exciton effects). An important aspect of possible experimental identification of these states is a gap in the excitation spectrum (the BCS gap in the case of a polaritonic BCS state). Similar to the polaritonic BCS gap, a light-induced gap can exist in photon lasers. Although polaritonic BCS states have been observed on the basis of spectroscopy in the vicinity…
Twisted two-dimensional bi-layers offer exquisite control on the electronic bandstructure through the interlayer rotation and coupling, enabling magic-angle flat-band superconductivity and moiré excitons. Here, we demonstrate how analogous principles, combined with large anisotropy, enable extreme control and manipulation of the photonic dispersion of phonon polaritons (PhPs) in van der Waals (vdW) bi-layers. We experimentally observe tunable topological transitions from open (hyperbolic) to closed (elliptic) dispersion contours in twisted bi-layered α-MoO3 at photonic magic angles, induced by…
van der Waals nanomaterials supporting phonon polariton quasiparticles possess unprecedented light confinement capabilities, making them ideal systems for molecular sensing, thermal emission, and subwavelength imaging applications, but they require defect-free crystallinity and nanostructured form factors to fully showcase these capabilities. We introduce bottom-up-synthesized α-MoO3 structures as nanoscale phonon polaritonic systems that feature tailorable morphologies and crystal qualities consistent with bulk single crystals. α-MoO3 nanoribbons serve as low-loss hyperbolic Fabry-Pérot nanor…
Phonon polaritons (PhPs),light coupled to lattice vibrations,with in-plane hyperbolic dispersion exhibit ray-like propagation with large wavevectors and enhanced density of optical states along certain directions on a surface. As such, they have raised a surge of interest as they promise unprecedented possibilities for the manipulation of infrared light with planar circuitry and at the nanoscale. Here, we demonstrate, for the first time, the focusing of in-plane hyperbolic PhPs propagating along thin slabs of MoO3. To that end, we developed metallic nanoantennas of convex geometries for both t…
Van der Waals materials and heterostructures manifesting strongly bound room temperature exciton states exhibit emergent physical phenomena and are of a great promise for optoelectronic applications. Here, we demonstrate that nanostructured multilayer transition metal dichalcogenides by themselves provide an ideal platform for excitation and control of excitonic modes, paving the way to exciton-photonics. Hence, we show that by patterning the TMDCs into nanoresonators, strong dispersion and avoided crossing of excitons and hybrid polaritons with interaction potentials exceeding 410 meV may be …
We show that planar semiconductor microcavities in the strong coupling regime can be used as sources of stimulated terahertz (THz) radiation. Emitted THz photons would have a frequency of the spliting of the cavity polariton modes. The optical transition between upper and lower polariton branches is allowed due to mixing of the upper polariton state with one of excited exciton states. This transition is stimulated in the polariton laser regime.
Van der Waals heterostructures assembled from layers of 2D materials have attracted considerable interest due to their novel optical and electrical properties. Here we report a scattering-type scanning near field optical microscopy study of hexagonal boron nitride on black phosphorous (h-BN/BP) heterostructures, demonstrating the first direct observation of in-plane anisotropic phonon polariton modes in vdW heterostructures. Strikingly, the measured in-plane optical anisotropy along armchair and zigzag crystal axes exceeds the ratio of refractive indices of BP in the x-y plane. We explain that…
Twisted atomically thin semiconductors are characterized by moiré excitons. Their optical signatures and selection rules are well understood. However, their hybridization with photons in the strong coupling regime for heterostructures integrated in an optical cavity has not been in the focus of research yet. Here, we combine an excitonic density matrix formalism with a Hopfield approach to provide microscopic insights into moiré exciton polaritons. In particular, we show that exciton-light coupling, polariton energy, and even the number of polariton branches can be controlled via the twist ang…
We theoretically investigate the application of topological plasmon polaritons (TPPs) to temperature sensing for the first time. Based on an analogy of the topological edge states in the Su-Schrieffer-Heeger model, TPPs are realized in a one-dimensional intrinsic indium antimonide (InSb) microsphere chain. The existence of TPPs is demonstrated by analyzing the topology of the photonic band structures and the eigenmode distribution. By exploiting the temperature dependence of the permittivity of InSb in the terahertz range, the resonance frequency of the TPPs can be largely tuned by the tempera…
Van der Waals (vdW) materials exhibit intriguing structural, electronic and photonic properties. Electron Energy Loss Spectroscopy (EELS) within Scanning Transmission Electron Microscope (STEM) allows for nanoscale mapping of such properties. However, typical STEM-EELS detection is limited to energy losses in the eV range, which are too large for probing important low-energy excitation such as phonons or mid-IR plasmons. Here we adapt a conventional STEM-EELS system to probe energy loss down to 100 meV, and apply it to map phononic states in h-BN, a representative van der Waals (vdW) material.…
yperbolic polaritons in van der Waals materials recently attract a lot of attention, owing to their strong electromagnetic field confinement, ultraslow group velocities and long lifetimes. Typically, volume confined hyperbolic polaritons (HPs) are studied. Here we show the first near-field optical images of hyperbolic surface polarities, HSPs, which are confined and guided at the edges of thin flakes of a vdW material. To that end, we applied scattering-type scanning near-field optical microscopy (s-SNOM) for launching and real-space nanoimaging of hyperbolic surface phonon polariton modes on …
Strong coupling between magnon and electromagnetic wave can lead to the formation of a coupled spinphoton quasiparticle named as magnon-polariton. The phenomenon is well studied for ferromagnetic systems inside microwave cavities in recent years. However, formation of magnon-polariton is rarely seen for an antiferromagnet (AFM) because the strong coupling condition is not easily fulfilled. Here we present time-domain terahertz measurement on a multiferroic polar antiferromagnet Fe2Mo3O8. We find clearly beating between two modes at frequencies above and below the electric-active magnon frequen…
We analyze theoretically the spin dynamics of exciton-polaritons and photons during their Bloch oscillations in a one-dimensional microwire. The wire geometry induces an energy splitting between the longitudinal and transverse electric polarized eigenmodes. We show analytically that a synchronized regime between the Bloch oscillations in space and the precession of the pseudospin can be achieved. This synchronization results in the formation of a THz alternating spin current which can be extracted out of the confinement region by the Landau-Zener tunneling towards the second allowed miniband. …
Layered materials can be assembled vertically to fabricate a new class of van der Waals (VDW) heterostructures a few atomic layers thick, compatible with a wide range of substrates and optoelectronic device geometries, enabling new strategies for control of light-matter coupling. Here, we incorporate molybdenum diselenide/boron nitride (MoSe$_2$/hBN) quantum wells (QWs) in a tunable optical microcavity. Part-light-part-matter polariton eigenstates are observed as a result of the strong coupling between MoSe$_2$ excitons and cavity photons, evidenced from a clear anticrossing between the neutra…
We suggest an indirect method of detection of photons with zero projection of spin mediated by emission of terahertz photons. This terahertz source is based on a system of microcavity exciton polaritons in the regime of polariton BEC formation when the cavity photons acquire an effective mass being localised in the cavity and therefore receive the third spin degree of freedom (corresponding to the longitudinal polarization with chirality l = 0). The optical transitions can occur between two polariton ground states based on the light-hole and heavy-hole excitons, respectively, accompanied by th…
Optical nanoresonators are fundamental building blocks in a number of nanotechnology applications (e.g. in spectroscopy) due to their ability to efficiently confine light at the nanoscale. Recently, nanoresonators based on the excitation of phonon polaritons (PhPs) $-$ light coupled to lattice vibrations $-$ in polar crystals (e.g. SiC, or h-BN) have attracted much attention due to their strong field confinement, high-quality factors, and potential to enhance the photonic density of states at mid-infrared (IR) frequencies. Here, we go one step further by introducing PhPs nanoresonators that no…
Hyperbolic materials exhibit unique properties that enable a variety of intriguing applications in nanophotonics. The topological insulator Bi2Se3 represents a natural hyperbolic optical medium, both in the THz and visible range. Here, using cathodoluminescence spectroscopy and electron energy-loss spectroscopy, we demonstrate that Bi2Se3, in addition to being a hyperbolic material, supports room-temperature exciton polaritons. Moreover, we explore the behavior of hyperbolic edge exciton polaritons in Bi2Se3. Edge polaritons are hybrid modes that result from the coupling of the polaritons boun…
Dirac plasmons in graphene hybridize with phonons of transition metal dichalcogenides (TMDs) when the materials are combined in so-called van der Waals heterostructures (vdWh), thus forming surface plasmon-phonon polaritons (SPPPs). The extend to which these modes are coupled depends on the TMD composition and structure, but also on the plasmons' properties. By performing realistic simulations that account for the contribution of each layer of the vdWh separately, we calculate how the strength of plasmon-phonon coupling depends on the number and composition of TMD layers, on the graphene Fermi…
Vertical cavity surface emitting terahertz lasers can be realized in conventional semiconductor microcavities with embedded quantum wells in the strong coupling regime. The cavity is to be pumped optically at half the frequency of the 2p exciton state. Once a threshold population of 2p excitons is achieved, a stimulated terahertz transition populates the lower exciton-polariton branch, and the cavity starts emitting laser light both in the optical and terahertz ranges. The lasing threshold is sensitive to the statistics of photons of the pumping light.
Controlling matter-light interactions with cavities is of fundamental importance in modern science and technology. It is exemplified in the strong-coupling regime, where matter-light hybrid modes form, with properties controllable via the photon component on the optical-wavelength scale. In contrast, matter excitations on the nanometer scale are harder to access. In two-dimensional van der Waals heterostructures, a tunable moiré lattice potential for electronic excitations may form, enabling correlated electron gases in lattice potentials. Excitons confined in moiré lattices have also been rep…
The current (voltage) responsivity of the superlattice-based diode detectors in the terahertz frequency band which includes the region of the polar optical phonon frequencies has been analyzed theoretically. Within the framework of the equivalent circuit approach an electro-dynamical model which allows one to analyze the responsivity taking into account the plasmon polariton excitation both in the substrate and in the contact layers of the diodes has been suggested. It has been shown that the presence of the plasmon polariton excitation gives rise to strong features in the frequency dependence…
In this paper, we present a novel route to tunable spontaneous valley coherence in heterostructures of two dimensional valleytronic materials with other layered materials hosting anisotropic polaritonic modes. We first discuss the dependence of this coherence on the conductivity tensor of the anisotropic part of a general heterostructure and on its geometrical configuration. Subsequently, we propose two implementations - one, using anisotropic plasmons in phosphorene and another with hyperbolic phonon polaritons in MoO3. In both these systems we show for the first time electrostatic tunability…
Emergence of Propagating Exciton-Polaritons in Hybrid Waveguide-van der Waals Heterostructures
Institute of Physics, University of Rostock（罗斯托克大学物理研究所）；Ferdinand-Braun-Institut, Leibniz-Institut für Höchstfrequenztechnik (FBH)（费迪南德·布劳恩研究所，莱布尼茨高频技术研究所）；Research Center for Materials Nanoarchitectonics, NIMS（日本物质材料研究机构纳米结构材料研究中心）；Research Center for Electronic and Optical Materials, NIMS（日本物质材料研究机构电子光学材料研究中心）
