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Register a new userNanophotonics with 2D Transition Metal Dichalcogenides
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Two-dimensional transition metal dichalcogenides (TMDCs) have recently become attractive semiconductor materials for several optoelectronic applications, such as photodetection, light harvesting, phototransistors, light-emitting diodes, and lasers. They are particularly appealing because 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 nanophotonic devices. Here, we review state-of-the-art advances on hybrid exciton-polariton structures based on monolayer TMDCs coupled to plasmonic and dielectric nanocavities. We first generally discuss the optical properties of 2D WS2, WSe2, MoS2 and MoSe2 materials, paying special attention to their energy and photoluminescence/absorption spectra, excitonic fine structure, and to the dynamics of exciton formation and valley depolarization. We then discuss light-matter interactions in 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 based on this novel material platform.
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Monolayer transition metal dichalcogenides (TMDs) exhibit high nonlinear optical (NLO) susceptibilities. Experiments on MoS$_2$ have indeed revealed very large second-order ($chi^{(2)}$) and third-order ($chi^{(3)}$) optical susceptibilities. However, third harmonic generation results of other layered TMDs has not been reported. Furthermore, the reported $chi^{(2)}$ and $chi^{(3)}$ of MoS$_2$ vary by several orders of magnitude, and a reliable quantitative comparison of optical nonlinearities across different TMDs has remained elusive. Here, we investigate second- and third-harmonic generation, and three-photon photoluminescence in TMDs. Specifically, we present an experimental study of $chi^{(2)}$, and $chi^{(3)}$ of four common TMD materials (ce{MoS2}, ce{MoSe2}, ce{WS2} and ce{WSe2}) by placing different TMD flakes in close proximity to each other on a common substrate, allowing their NLO properties to be accurately obtained from a single measurement. $chi^{(2)}$ and $chi^{(3)}$ of the four monolayer TMDs have been compared, indicating that they exhibit distinct NLO responses. We further present theoretical simulations of these susceptibilities in qualitative agreement with the measurements. Our comparative studies of the NLO responses of different two-dimensional layered materials allow us to select the best candidates for atomic-scale nonlinear photonic applications, such as frequency conversion and all-optical signal processing.
Two dimensional (2D) transition metal dichalcogenide (TMDC) materials, such as MoS2, WS2, MoSe2, and WSe2, have received extensive attention in the past decade due to their extraordinary physical properties. The unique properties make them become ideal materials for various electronic, photonic and optoelectronic devices. However, their performance is limited by the relatively weak light-matter interactions due to their atomically thin form factor. Resonant nanophotonic structures provide a viable way to address this issue and enhance light-matter interactions in 2D TMDCs. Here, we provide an overview of this research area, showcasing relevant applications, including exotic light emission, absorption and scattering features. We start by overviewing the concept of excitons in 1L-TMDC and the fundamental theory of cavity-enhanced emission, followed by a discussion on the recent progress of enhanced light emission, strong coupling and valleytronics. The atomically thin nature of 1L-TMDC enables a broad range of ways to tune its electric and optical properties. Thus, we continue by reviewing advances in TMDC-based tunable photonic devices. Next, we survey the recent progress in enhanced light absorption over narrow and broad bandwidths using 1L or few-layer TMDCs, and their applications for photovoltaics and photodetectors. We also review recent efforts of engineering light scattering, e.g., inducing Fano resonances, wavefront engineering in 1L or few-layer TMDCs by either integrating resonant structures, such as plasmonic/Mie resonant metasurfaces, or directly patterning monolayer/few layers TMDCs. We then overview the intriguing physical properties of different types of van der Waals heterostructures, and their applications in optoelectronic and photonic devices. Finally, we draw our opinion on potential opportunities and challenges in this rapidly developing field of research.
The recently emerged concept of all-dielectric nanophotonics based on optical Mie resonances in high-index dielectric nanoparticles has proven 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.
Transition metal dichalcogenides (TMDs) represent an entire new class of semiconducting 2D materials with exciting properties. Defects in 2D TMDs can crucially affect their physical and chemical properties. However, characterization of the presence and spatial distribution of defects is limited either in throughput or in resolution. Here, we demonstrate large area mapping of reactive sulfur-deficient defects in 2D-TMDs coupling single-molecule localization microscopy with fluorescence labeling using thiol chemistry. Our method, reminiscent of PAINT strategies, relies on the specific binding by reversible physisorption of fluorescent probes to sulfur-vacancies via a thiol group and their intermittent emission to apply localization of the labeled defects with a precision down to 15 nm. Tuning the distance between the fluorophore and the docking thiol site allows us to control Foster Resonance Energy Transfer (FRET) process and reveal large structural defects such as grain boundaries and line defects, due to the local irregular lattice structure. Our methodology provides a simple and fast alternative for large-scale mapping of non-radiative defects in 2D materials and paves the way for in-situ and spatially resolved monitoring of the interaction between chemical agent and the defects in 2D materials that has general implications for defect engineering in aqueous condition.
Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here we review recent progress in our understanding of the excitonic properties in monolayer TMDs and lay out future challenges. We focus on the consequences of the strong direct and exchange Coulomb interaction, discuss exciton-light interaction and effects of other carriers and excitons on electron-hole pairs in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized.
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