Enhanced second-order nonlinearities at strained ultrasharp zigzag edges in multilayer MoS2

Transition metal dichalcogenide (TMD) materials attract significant research attention thanks to their exceptional excitonic and optical properties. In this work, we analyze the formation of strained ultrasharp zigzag edges in MoS2 multilayers produced by anisotropic wet etching. The topography of the edges is determined by the relative stability of the different crystallographic directions of the multilayer as well as the interlayer interactions. Furthermore, we study the linear (Raman) and nonlinear (second-harmonic generation) spectroscopic characteristics of such edges and observe enhanced second-order nonlinearity originating from the strained zigzag edges. We also confirm that ultrasharp hexagonal nanoholes in MoS2 grow along the most stable crystallographic directions despite potential stacking faults or instabilities in the crystal quality. Our results open the way to exploit a broad range of phenomena occurring at the edges of MoS2 material, including the unique determination of crystal orientation for moiré engineering and strongly correlated phenomena in 2D material-based systems, as well as potential applications in TMD-based electrocatalysis and gas sensing

Dimer-on-mirror SERS substrates with attogram sensitivity fabricated by colloidal lithography

Nanoplasmonic substrates with optimized field-enhancement properties are a key component in the continued development of surface-enhanced Raman scattering (SERS) molecular analysis but are challenging to produce inexpensively in large scale. We used a facile and cost-effective bottom-up technique, colloidal hole-mask lithography, to produce macroscopic dimer-on-mirror gold nanostructures. The optimized structures exhibit excellent SERS performance, as exemplified by detection of 2.5 and 50 attograms of BPE, a common SERS probe, using Raman microscopy and a simple handheld device, respectively. The corresponding Raman enhancement factor is of the order 10(11), which compares favourably to previously reported record performance values

Self-hybridized vibrational-Mie polaritons in water droplets

We study the self-hybridization between Mie modes supported by water droplets with stretching and bending vibrations in water molecules. Droplets with radii $>2.7~\mu m$ are found to be polaritonic on the onset of the ultrastrong light-matter coupling regime. Similarly, the effect is observed in larger deuterated water droplets at lower frequencies. Our results indicate that polaritonic states are ubiquitous in nature and occur in water droplets in mists, fogs, and clouds. This finding may have implications not only for polaritonic physics but also for aerosol and atmospheric sciences.Comment: Main text: 6 pages, 3 figures. Supplemental: 9 pages, 8 figure

Polaritonic linewidth asymmetry in the strong and ultrastrong coupling regime

The intriguing properties of polaritons resulting from strong and ultrastrong light–matter coupling have been extensively investigated. However, most research has focused on spectroscopic characteristics of polaritons, such as their eigenfrequencies and Rabi splitting. Here, we study the decay rates of a plasmon–microcavity system in the strong and ultrastrong coupling regimes experimentally and numerically. We use a classical scattering matrix approach, approximating our plasmonic system with an effective Lorentz model, to obtain the decay rates through the imaginary part of the complex quasinormal mode eigenfrequencies. Our classical model automatically includes all the interaction terms necessary to account for ultrastrong coupling without dealing with the rotating-wave approximation and the diamagnetic term. We find an asymmetry in polaritonic decay rates, which deviate from the expected average of the uncoupled system’s decay rates at zero detuning. Although this phenomenon has been previously observed in exciton–polaritons and attributed to their disorder, we observe it even in our homogeneous system. As the coupling strength of the plasmon–microcavity system increases, the asymmetry also increases and can become so significant that the lower (upper) polariton decay rate reduction (increase) goes beyond the uncoupled decay rates, γ − < γ 0,c < γ +. Furthermore, our findings demonstrate that polaritonic linewidth asymmetry is a generic phenomenon that persists even in the case of bulk polaritons

Probing optical anapoles with fast electron beams

Abstract Optical anapoles are intriguing charge-current distributions characterized by a strong suppression of electromagnetic radiation. They originate from the destructive interference of the radiation produced by electric and toroidal multipoles. Although anapoles in dielectric structures have been probed and mapped with a combination of near- and far-field optical techniques, their excitation using fast electron beams has not been explored so far. Here, we theoretically and experimentally analyze the excitation of optical anapoles in tungsten disulfide (WS2) nanodisks using Electron Energy Loss Spectroscopy (EELS) in Scanning Transmission Electron Microscopy (STEM). We observe prominent dips in the electron energy loss spectra and associate them with the excitation of optical anapoles and anapole-exciton hybrids. We are able to map the anapoles excited in the WS2 nanodisks with subnanometer resolution and find that their excitation can be controlled by placing the electron beam at different positions on the nanodisk. Considering current research on the anapole phenomenon, we envision EELS in STEM to become a useful tool for accessing optical anapoles appearing in a variety of dielectric nanoresonators