Enhanced Photon-Phonon Interaction in WSe2 Acoustic Nanocavities.

Acoustic nanocavities (ANCs) with resonance frequencies much above 1 GHz are prospective to be exploited in sensors and quantum operating devices. Nowadays, acoustic nanocavities fabricated from van der Waals (vdW) nanolayers allow them to exhibit resonance frequencies of the breathing acoustic mode up to f ∼ 1 THz and quality factors up to Q ∼ 103. For such high acoustic frequencies, electrical methods fail, and optical techniques are used for the generation and detection of coherent phonons. Here, we study experimentally acoustic nanocavities fabricated from WSe2 layers with thicknesses from 8 up to 130 nm deposited onto silica colloidal crystals. The substrate provides a strong mechanical support for the layers while keeping their acoustic properties the same as in membranes. We concentrate on experimental and theoretical studies of the amplitude of the optically measured acoustic signal from the breathing mode, which is the most important characteristic for acousto-optical devices. We probe the acoustic signal optically with a single wavelength in the vicinity of the exciton resonance and measure the relative changes in the reflectivity induced by coherent phonons up to 3 × 10-4 for f ∼ 100 GHz. We reveal the enhancement of photon-phonon interaction for a wide range of acoustic frequencies and show high sensitivity of the signal amplitude to the photoelastic constants governed by the deformation potential and dielectric function for photon energies near the exciton resonance. We also reveal a resonance in the photoelastic response (we call it photoelastic resonance) in the nanolayers with thickness close to the Bragg condition. The estimates show the capability of acoustic nanocavities with an exciton resonance for operations with high-frequency single phonons at an elevated temperature.

Giant Ultrafast All-Optical Modulation Based on Exceptional Points in Exciton-Polariton Perovskite Metasurfaces.

Ultrafast all-optical modulation with optically resonant nanostructures is an essential technology for high-speed signal processing on a compact optical chip. Key challenges that exist in this field are relatively low and slow modulations in the visible range as well as the use of expensive materials. Here we develop an ultrafast all-optical modulator based on MAPbBr3 perovskite metasurface supporting exciton-polariton states with exceptional points. The additional angular and spectral filtering of the modulated light transmitted through the designed metasurface allows us to achieve 2500% optical signal modulation with the shortest modulation time of 440 fs at the pump fluence of ∼40 µJ/cm2. Such a value of the modulation depth is record-high among the existing modulators in the visible range, while the main physical effect behind it is polariton condensation. Scalable and cheap metasurface fabrication via nanoimprint lithography along with the simplicity of perovskite synthesis and deposition make the developed approach promising for real-life applications.

Probing and Control of Guided Exciton-Polaritons in a 2D Semiconductor-Integrated Slab Waveguide.

Guided 2D exciton-polaritons, resulting from the strong coupling of excitons in semiconductors with nonradiating waveguide modes, provide an attractive approach toward developing novel on-chip optical devices. These quasiparticles are characterized by long propagation distances and efficient nonlinear interactions but cannot be directly accessed from the free space. Here we demonstrate a powerful approach for probing and manipulating guided polaritons in a Ta2O5 slab integrated with a WS2 monolayer using evanescent coupling through a high-index solid immersion lens. Tuning the nanoscale lens-sample gap allows for extracting all of the intrinsic parameters of the system. We also demonstrate the transition from weak to strong coupling accompanied by the onset of the motional narrowing effect: with the increase of exciton-photon coupling strength, the inhomogeneous contribution to polariton line width, inherited from the exciton resonance, becomes fully lifted. Our results enable the development of integrated optics employing room-temperature exciton-polaritons in 2D semiconductor-based structures.

Coherent Phonons in van der Waals MoSe2/WSe2 Heterobilayers.

The increasing role of two-dimensional (2D) devices requires the development of new techniques for ultrafast control of physical properties in 2D van der Waals (vdW) nanolayers. A special feature of heterobilayers assembled from vdW monolayers is femtosecond separation of photoexcited electrons and holes between the neighboring layers, resulting in the formation of Coulomb force. Using laser pulses, we generate a 0.8 THz coherent breathing mode in MoSe2/WSe2 heterobilayers, which modulates the thickness of the heterobilayer and should modulate the photogenerated electric field in the vdW gap. While the phonon frequency and decay time are independent of the stacking angle between the MoSe2 and WSe2 monolayers, the amplitude decreases at intermediate angles, which is explained by a decrease in the photogenerated electric field between the layers. The modulation of the vdW gap by coherent phonons enables a new technology for the generation of THz radiation in 2D nanodevices with vdW heterobilayers.

Polaron-Enhanced Polariton Nonlinearity in Lead Halide Perovskites.

Exciton-polaritons offer a versatile platform for realization of all-optical integrated logic gates due to the strong effective optical nonlinearity resulting from the exciton-exciton interactions. In most of the current excitonic materials there exists a direct connection between the exciton robustness to thermal fluctuations and the strength of the exciton-exciton interaction, making materials with the highest levels of exciton nonlinearity applicable at cryogenic temperatures only. Here, we show that strong polaronic effects, characteristic for perovskite materials, allow overcoming this limitation. Namely, we demonstrate a record-high value of the nonlinear optical response in the nanostructured organic-inorganic halide perovskite MAPbI3, experimentally detected as a 19.7 meV blueshift of the polariton branch under femtosecond laser irradiation. This is substantially higher than characteristic values for the samples based on conventional semiconductors and monolayers of transition-metal dichalcogenides. The observed strong polaron-enhanced nonlinearity exists for both tetragonal and orthorhombic phases of MAPbI3 and remains stable at elevated temperatures.

Nanoscale Electrically Driven Light Source Based on Hybrid Semiconductor/Metal Nanoantenna.

A micro- or nanosized electrically controlled source of optical radiation is one of the key elements in optoelectronic systems. The phenomenon of light emission via inelastic tunneling (LEIT) of electrons through potential barriers or junctions opens up new possibilities for development of such sources. In this work, we present a simple approach for fabrication of nanoscale electrically driven light sources based on LEIT. We employ STM lithography to locally modify the surface of a Si/Au film stack via heating, which is enabled by a high-density tunnel current. Using the proposed technique, hybrid Si/Au nanoantennas with a minimum diameter of 60 nm were formed. Studying both electronic and optical properties of the obtained nanoantennas, we confirm that the resulting structures can efficiently emit photons in the visible range because of inelastic scattering of electrons. The proposed approach allows for fabrication of nanosized hybrid nanoantennas and studying their properties using STM.

Experimental observation of topological Z2 exciton-polaritons in transition metal dichalcogenide monolayers.

The rise of quantum science and technologies motivates photonics research to seek new platforms with strong light-matter interactions to facilitate quantum behaviors at moderate light intensities. Topological polaritons (TPs) offer an ideal platform in this context, with unique properties stemming from resilient topological states of light strongly coupled with matter. Here we explore polaritonic metasurfaces based on 2D transition metal dichalcogenides (TMDs) as a promising platform for topological polaritonics. We show that the strong coupling between topological photonic modes of the metasurface and excitons in TMDs yields a topological polaritonic Z2 phase. We experimentally confirm the emergence of one-way spin-polarized edge TPs in metasurfaces integrating MoSe2 and WSe2. Combined with the valley polarization in TMD monolayers, the proposed system enables an approach to engage the photonic angular momentum and valley and spin of excitons, offering a promising platform for photonic/solid-state interfaces for valleytronics and spintronics.

Scanning Tunneling Microscopy-Induced Light Emission and I(V) Study of Optical Near-Field Properties of Single Plasmonic Nanoantennas.

Electrically driven plasmonic nanoantennas can be integrated as a local source of the optical signal of advanced photonic schemes for on-chip data processing. The inelastic electron tunneling provides the photon generation or launch of surface plasmon waves. This process can be enhanced by the local density of optical states of nanoantennas. In this paper, we used scanning tunnel microscopy-induced light emission to probe the local optoelectronic properties of single gold nanodiscs. The electromagnetic field distribution in the vicinity of plasmonic structures was investigated with high spatial resolution. The obtained photon maps reveal the nonuniform distribution of electromagnetic near-fields, which is consistent with nanoantenna optical modes. Also, the analysis of derived I(V) curves showed a direct correlation between the nanoantenna optical states and the appearance of features on current-voltage characteristics.

Nonlinear polaritons in a monolayer semiconductor coupled to optical bound states in the continuum.

Optical bound states in the continuum (BICs) provide a way to engineer very narrow resonances in photonic crystals. The extended interaction time in these systems is particularly promising for the enhancement of nonlinear optical processes and the development of the next generation of active optical devices. However, the achievable interaction strength is limited by the purely photonic character of optical BICs. Here, we mix the optical BIC in a photonic crystal slab with excitons in the atomically thin semiconductor MoSe2 to form nonlinear exciton-polaritons with a Rabi splitting of 27 meV, exhibiting large interaction-induced spectral blueshifts. The asymptotic BIC-like suppression of polariton radiation into the far field toward the BIC wavevector, in combination with effective reduction of the excitonic disorder through motional narrowing, results in small polariton linewidths below 3 meV. Together with a strongly wavevector-dependent Q-factor, this provides for the enhancement and control of polariton-polariton interactions and the resulting nonlinear optical effects, paving the way toward tuneable BIC-based polaritonic devices for sensing, lasing, and nonlinear optics.

Effective surface conductivity of optical hyperbolic metasurfaces: from far-field characterization to surface wave analysis.

Metasurfaces offer great potential to control near- and far-fields through engineering optical properties of elementary cells or meta-atoms. Such perspective opens a route to efficient manipulation of the optical signals both at nanoscale and in photonics applications. In this paper we show that a local surface conductivity tensor well describes optical properties of a resonant plasmonic hyperbolic metasurface both in the far-field and in the near-field regimes, where spatial dispersion usually plays a crucial role. We retrieve the effective surface conductivity tensor from the comparative analysis of experimental and numerical reflectance spectra of a metasurface composed of elliptical gold nanoparticles. Afterwards, the restored conductivities are validated by semi-analytic parameters obtained with the nonlocal discrete dipole model with and without interaction contribution between meta-atoms. The effective parameters are further used for the dispersion analysis of surface plasmons localized at the metasurface. The obtained effective conductivity describes correctly the dispersion law of both quasi-TE and quasi-TM plasmons in a wide range of optical frequencies as well as the peculiarities of their propagation regimes, in particular, topological transition from the elliptical to hyperbolic regime with eligible accuracy. The analysis in question offers a simple practical way to describe properties of metasurfaces including ones in the near-field zone with effective conductivity tensor extracting from the convenient far-field characterization.

Microwave platform as a valuable tool for characterization of nanophotonic devices.

The rich potential of the microwave experiments for characterization and optimization of optical devices is discussed. While the control of the light fields together with their spatial mapping at the nanoscale is still laborious and not always clear, the microwave setup allows to measure both amplitude and phase of initially determined magnetic and electric field components without significant perturbation of the near-field. As an example, the electromagnetic properties of an add-drop filter, which became a well-known workhorse of the photonics, is experimentally studied with the aid of transmission spectroscopy measurements in optical and microwave ranges and through direct mapping of the near fields at microwave frequencies. We demonstrate that the microwave experiments provide a unique platform for the comprehensive studies of electromagnetic properties of micro- and nanophotonic devices, and allow to obtain data which are hardly acquirable by conventional optical methods.

Resonant Raman scattering from silicon nanoparticles enhanced by magnetic response.

Enhancement of optical response with high-index dielectric nanoparticles is attributed to the excitation of their Mie-type magnetic and electric resonances. Here we study Raman scattering from crystalline silicon nanoparticles and reveal that magnetic dipole modes have a much stronger effect on the scattering than electric modes of the same order. We demonstrate experimentally a 140-fold enhancement of the Raman signal from individual silicon spherical nanoparticles at the magnetic dipole resonance. Our results confirm the importance of the optically-induced magnetic response of subwavelength dielectric nanoparticles for enhancing light-matter interactions.

Enhancement of artificial magnetism via resonant bianisotropy.

All-dielectric "magnetic light" nanophotonics based on high refractive index nanoparticles allows controlling magnetic component of light at nanoscale without having high dissipative losses. The artificial magnetic optical response of such nanoparticles originates from circular displacement currents excited inside those structures and strongly depends on geometry and dispersion of optical materials. Here an approach for enhancing of magnetic response via resonant bianisotropy effect is proposed and analyzed. The key mechanism of enhancement is based on electric-magnetic interaction between two electrically and magnetically resonant nanoparticles of all-dielectric dimer. It was shown that proper geometrical arrangement of the dimer in respect to the incident illumination direction allows flexible control over all vectorial components of the magnetic moment, tailoring the latter in the dynamical range of 100% and delivering enhancement up to 36% relative to performances of standalone spherical particles. The proposed approach provides pathways for designs of all-dielectric metamaterials and metasurfaces with strong magnetic responses.

Mapping plasmonic topological states at the nanoscale.

We report on the first experimental observation of topological edge states in zigzag chains of plasmonic nanodisks. We demonstrate that such edge states can be selectively excited with the linear polarization of the incident light, and visualize them directly by near-field scanning optical microscopy. Our work provides experimental verification of a novel paradigm for manipulating light at the nanoscale in topologically nontrivial structures.

Magnetic and electric hotspots with silicon nanodimers.

The study of the resonant behavior of silicon nanostructures provides a new route for achieving efficient control of both electric and magnetic components of light. We demonstrate experimentally and numerically that enhancement of localized electric and magnetic fields can be achieved in a silicon nanodimer. For the first time, we experimentally observe hotspots of the magnetic field at visible wavelengths for light polarized across the nanodimer's primary axis, using near-field scanning optical microscopy.

Demonstration of unusual nanoantenna array modes through direct reconstruction of the near-field signal.

We perform complex investigation of the distribution of electromagnetic fields in the vicinity of an array of silver nanoantennas, which can operate as an efficient light trapping structure in the visible spectral range. In theory, this array should support unusual collective modes that possess an advantageous distribution of local electric fields, ensuring both strong field localization beneath nanoantennas and a low level of optical losses inside the metal. Using an aperture-type near-field scanning optical microscope (NSOM), we obtain near-field patterns that show excellent agreement with the NSOM signal, directly reconstructed from rigorous numerical simulations using an approach based on the electromagnetic reciprocity theorem. The agreement between theory and experiment allows us to claim the first-time experimental verification of the existence of collective modes with such properties in an array of silver nanoantennas. The confirmation of this physical phenomenon opens the door to a new class of light-trapping structures for photovoltaics.

Nanoscale patterning of metal nanoparticle distribution in glasses.

: We show that electric field imprinting technique allows for patterning of metal nanoparticles in the glass matrix at the subwavelength scale. The formation of glass-metal nanocomposite strips with a width down to 150 nm is demonstrated. The results of near-field microscopy of imprinted patterns are in good agreement with the performed numerical modeling. Atomic force microscopy reveals that imprinting also results in the formation of nanoscale surface profile with the height going down with the decrease of the strip width. The experiments prove the applicability of this technique for the fabrication of nanoscale plasmonic components.