Indirect bandgap MoSe2 resonators for light-emitting nanophotonics.

Transition metal dichalcogenides (TMDs) are promising for new generation nanophotonics due to their unique optical properties. However, in contrast to direct bandgap TMD monolayers, bulk samples have an indirect bandgap that restricts their application as light emitters. On the other hand, the high refractive index of these materials allows for effective light trapping and the creation of high-Q resonators. In this work, a method for the nanofabrication of microcavities from indirect TMD multilayer flakes, which makes it possible to achieve pronounced resonant photoluminescence enhancement due to the cavity modes, is proposed. Whispering gallery mode (WGM) resonators are fabricated from bulk indirect MoSe2 using resistless scanning probe lithography. A micro-photoluminescence (µ-PL) investigation revealed the WGM spectra of the resonators with an enhancement factor up to 100. The characteristic features of WGMs are clearly seen from the scattering experiments which are in agreement with the results of numerical simulations. It is shown that the PL spectra in the fabricated microcavities are contributed by two mechanisms demonstrating different temperature dependences. The indirect PL, which is quenched with the temperature decrease, and the direct PL which almost does not depend on the temperature. The results of the work show that the suggested approach has great prospects in nanophotonics.

Beyond Bounds on Light Scattering with Complex Frequency Excitations.

Light scattering is one of the most established wave phenomena in optics, lying at the heart of light-matter interactions and of crucial importance for nanophotonic applications. Passivity, causality, and energy conservation imply strict bounds on the degree of control over scattering from small particles, with implications on the performance of many optical devices. Here, we demonstrate that these bounds can be surpassed by considering excitations at complex frequencies, yielding extreme scattering responses as tailored nanoparticles reach a quasi-steady-state regime. These mechanisms can be used to engineer light scattering of nanostructures beyond conventional limits for noninvasive sensing, imaging, and nanoscale light manipulation.

Suppressing material loss in the visible and near-infrared range for functional nanophotonics using bandgap engineering.

All-dielectric nanostructures have recently opened exciting opportunities for functional nanophotonics, owing to their strong optical resonances along with low material loss in the near-infrared range. Pushing these concepts to the visible range is hindered by their larger absorption coefficient, thus encouraging the search for alternative dielectrics for nanophotonics. Here, we employ bandgap engineering to synthesize hydrogenated amorphous Si nanoparticles (a-Si:H NPs) offering ideal features for functional nanophotonics. We observe significant material loss suppression in a-Si:H NPs in the visible range caused by hydrogenation-induced bandgap renormalization, producing strong higher-order resonant modes in single NPs with Q factors up to ~100 in the visible and near-IR range. We also realize highly tunable all-dielectric meta-atoms by coupling a-Si:H NPs to photochromic spiropyran molecules. ~70% reversible all-optical tuning of light scattering at the higher-order resonant mode under a low incident light intensity is demonstrated. Our results promote the development of high-efficiency visible nanophotonic devices.

All-optical reconfigurable chiral meta-molecules.

Chirality is a ubiquitous phenomenon in the natural world. Many biomolecules without inversion symmetry such as amino acids and sugars are chiral molecules. Measuring and controlling molecular chirality at a high precision down to the atomic scale are highly desired in physics, chemistry, biology, and medicine, however, have remained challenging. Herein, we achieve all-optical reconfigurable chiral meta-molecules experimentally using metallic and dielectric colloidal particles as artificial atoms or building blocks to serve at least two purposes. One is that the on-demand meta-molecules with strongly enhanced optical chirality are well-suited as substrates for surface-enhanced chiroptical spectroscopy of chiral molecules and as active components in optofluidic and nanophotonic devices. The other is that the bottom-up-assembled colloidal meta-molecules provide microscopic models to better understand the origin of chirality in the actual atomic and molecular systems.

Enhanced excitation and emission from 2D transition metal dichalcogenides with all-dielectric nanoantennas.

The recently emerged concept of all-dielectric nanophotonics based on optical Mie resonances in high-index dielectric nanoparticles has proven to be a promising pathway to boost light-matter interactions at the nanoscale. In this work, we discuss the opportunities enabled by the interaction of dielectric nanoresonators with 2D transition metal dichalcogenides (2D TMDCs), leading to weak and strong coupling regimes. We perform a comprehensive analysis of bright exciton photoluminescence (PL) enhancement from various 2D TMDCs, including WS2, MoS2, WSe2, and MoSe2 via their coupling to Mie resonances of a silicon nanoparticle. For each case, we find the system parameters corresponding to maximal PL enhancement taking into account excitation rate, Purcell factor and radiation efficiency. We demonstrate numerically that all-dielectric Si nanoantennas can significantly enhance the PL intensity from 2D TMDC by a factor of hundred through precise optimization of the geometrical and material parameters. Our results may be useful for high-efficiency 2D TMDC-based optoelectronic, nanophotonic, and quantum optical devices.

Asymmetric Metasurfaces with High-Q Resonances Governed by Bound States in the Continuum.

We reveal that metasurfaces created by seemingly different lattices of (dielectric or metallic) meta-atoms with broken in-plane symmetry can support sharp high-Q resonances arising from a distortion of symmetry-protected bound states in the continuum. We develop a rigorous theory of such asymmetric periodic structures and demonstrate a link between the bound states in the continuum and Fano resonances. Our results suggest the way for smart engineering of resonances in metasurfaces for many applications in nanophotonics and metaoptics.

Nanophotonics with 2D transition metal dichalcogenides [Invited].

Two-dimensional semiconducting transition metal dichalcogenides (TMDCs) have recently become attractive materials for several optoelectronic applications, such as photodetection, light harvesting, phototransistors, light-emitting diodes, and lasers. Their bandgap lies in the visible and near-IR range, and they possess strong excitonic resonances, high oscillator strengths, and valley-selective response. Coupling these materials to optical nanocavities enhances the quantum yield of exciton emission, enabling advanced quantum optics and nanophotonics devices. Here, we review the state-of-the-art advances of hybrid exciton-polariton structures based on monolayer TMDCs coupled to plasmonic and dielectric nanocavities. We discuss the optical properties of 2D WS2, WSe2, MoS2 and MoSe2 materials, paying special attention to their energy bands, photoluminescence/absorption spectra, excitonic fine structure, and to the dynamics of exciton formation and valley depolarization. We also discuss light-matter interactions in such hybrid exciton-polariton structures. Finally, we focus on weak and strong coupling regimes in monolayer TMDCs-based exciton-polariton systems, envisioning research directions and future opportunities for this material platform.

Boosting Terahertz Photoconductive Antenna Performance with Optimised Plasmonic Nanostructures.

Advanced nanophotonics penetrates into other areas of science and technology, ranging from applied physics to biology, which results in many fascinating cross-disciplinary applications. It has been recently demonstrated that suitably engineered light-matter interactions at the nanoscale can overcome the limitations of today's terahertz (THz) photoconductive antennas, making them one step closer to many practical implications. Here, we push forward this concept by comprehensive numerical optimization and experimental investigation of a log-periodic THz photoconductive antenna coupled to a silver nanoantenna array. We shed light on the operation principles of the resulting hybrid THz antenna, providing an approach to boost its performance. By tailoring the size of silver nanoantennas and their arrangement, we obtain an enhancement of optical-to-THz conversion efficiency 2-fold larger compared with previously reported results for similar structures, and the strongest enhancement is around 1 THz, a frequency range barely achievable by other compact THz sources. We also propose a cost-effective fabrication procedure to realize such hybrid THz antennas with optimized plasmonic nanostructures via thermal dewetting process, which does not require any post processing and makes the proposed solution very attractive for applications.

Tunable Resonance Coupling in Single Si Nanoparticle-Monolayer WS2 Structures.

Two-dimensional semiconducting transition metal dichalcogenides (TMDCs) are extremely attractive materials for optoelectronic applications in the visible and near-infrared range. Coupling these materials to optical nanocavities enables advanced quantum optics and nanophotonic devices. Here, we address the issue of resonance coupling in hybrid exciton-polariton structures based on single Si nanoparticles (NPs) coupled to monolayer (1L)-WS2. We predict a strong coupling regime with a Rabi splitting energy exceeding 110 meV for a Si NP covered by 1L-WS2 at the magnetic optical Mie resonance because of the symmetry of the mode. Further, we achieve a large enhancement in the Rabi splitting energy up to 208 meV by changing the surrounding dielectric material from air to water. The prediction is based on the experimental estimation of TMDC dipole moment variation obtained from the measured photoluminescence spectra of 1L-WS2 in different solvents. An ability of such a system to tune the resonance coupling is realized experimentally for optically resonant spherical Si NPs placed on 1L-WS2. The Rabi splitting energy obtained for this scenario increases from 49.6 to 86.6 meV after replacing air by water. Our findings pave the way to develop high-efficiency optoelectronic, nanophotonic, and quantum optical devices.