Super-Resolution Exciton Imaging of Nanobubbles in 2D Semiconductors with Near-Field Nanophotoluminescence Microscopy.

Two-dimensional (2D) semiconductors, such as transition metal dichalcogenides, have emerged as important candidate materials for next-generation chip-scale optoelectronic devices with the development of large-scale production techniques, such as chemical vapor deposition (CVD). However, 2D materials need to be transferred to other target substrates after growth, during which various micro- and nanoscale defects, such as nanobubbles, are inevitably generated. These nanodefects not only influence the uniformity of 2D semiconductors but also may significantly alter the local optoelectronic properties of the composed devices. Hence, super-resolution discrimination and characterization of nanodefects are highly demanded. Here, we report a near-field nanophotoluminescence (nano-PL) microscope that can quickly screen nanobubbles and investigate their impact on local excitonic properties of 2D semiconductors by directly visualize the PL emission distribution with a very high spatial resolution of ∼10 nm, far below the optical diffraction limit, and a high speed of 10 ms/point under ambient conditions. By using nano-PL microscopy to map the exciton and trion emission intensity distributions in transferred CVD-grown monolayer tungsten disulfide (1L-WS2) flakes, it is found that the PL intensity decreases by 13.4% as the height of the nanobubble increases by every nanometer, which is mainly caused by the suppression of trion emission due to the strong doping effect from the substrate. In addition to the nanobubbles, other types of nanodefects, such as cracks, stacks, and grain boundaries, can also be characterized. The nano-PL method is proven to be a powerful tool for the nondestructive quality inspection of nanodefects as well as the super-resolution exploration of local optoelectronic properties of 2D materials.

Terahertz Twistoptics-Engineering Canalized Phonon Polaritons.

The terahertz (THz) frequency range is key to studying collective excitations in many crystals and organic molecules. However, due to the large wavelength of THz radiation, the local probing of these excitations in smaller crystalline structures or few-molecule arrangements requires sophisticated methods to confine THz light down to the nanometer length scale, as well as to manipulate such a confined radiation. For this purpose, in recent years, taking advantage of hyperbolic phonon polaritons (HPhPs) in highly anisotropic van der Waals (vdW) materials has emerged as a promising approach, offering a multitude of manipulation options, such as control over the wavefront shape and propagation direction. Here, we demonstrate the THz application of twist-angle-induced HPhP manipulation, designing the propagation of confined THz radiation between 8.39 and 8.98 THz in the vdW material α-molybdenum trioxide (α-MoO3), hence extending twistoptics to this intriguing frequency range. Our images, recorded by near-field optical microscopy, show the frequency- and twist-angle-dependent changes between hyperbolic and elliptic polariton propagation, revealing a polaritonic transition at THz frequencies. As a result, we are able to allocate canalization (highly collimated propagation) of confined THz radiation by carefully adjusting these two parameters, i.e. frequency and twist angle. Specifically, we report polariton canalization in α-MoO3 at 8.67 THz for a twist angle of 50°. Our results demonstrate the precise control and manipulation of confined collective excitations at THz frequencies, particularly offering possibilities for nanophotonic applications.

Plasmonic Nonlinear Energy Transfer Enhanced Second Harmonic Generation Nanoscopy.

Nonlinear optical response is a fingerprint of various physicochemical properties of materials related to symmetry, including crystallography, interfacial configuration, and carrier dynamics. However, the intrinsically weak nonlinear optical susceptibility and the diffraction limit of far-field optics restrict probing deep-subwavelength-scale nonlinear optics with measurable signal-to-noise ratio. Here, we propose an alternative approach toward efficient second harmonic generation (SHG) nanoscopy for SHG-active sample (zinc oxide nanowire; ZnO NW) using an SHG-active plasmonic nanotip. Our full-wave simulation suggests that the experimentally observed high near-field SHG contrast is possible when the nonlinear response of ZnO NW is enhanced and/or that of the tip is suppressed. This result suggests possible evidence of quantum mechanical nonlinear energy transfer between the tip and the sample, modifying the nonlinear optical susceptibility. Further, this process probes the nanoscale corrosion of ZnO NW, demonstrating potential use in studying various physicochemical phenomena in nanoscale resolution.

Germanium Monosulfide as a Natural Platform for Highly Anisotropic THz Polaritons.

Terahertz (THz) electromagnetic radiation is key to access collective excitations such as magnons (spins), plasmons (electrons), or phonons (atomic vibrations), thus bridging topics between optics and solid-state physics. Confinement of THz light to the nanometer length scale is desirable for local probing of such excitations in low-dimensional systems, thereby circumventing the large footprint and inherently low spectral power density of far-field THz radiation. For that purpose, phonon polaritons (PhPs) in anisotropic van der Waals (vdW) materials have recently emerged as a promising platform for THz nanooptics. Hence, there is a demand for the exploration of materials that feature not only THz PhPs at different spectral regimes but also host anisotropic (directional) electrical, thermoelectric, and vibronic properties. To that end, we introduce here the semiconducting vdW-material alpha-germanium(II) sulfide (GeS) as an intriguing candidate. By employing THz nanospectroscopy supported by theoretical analysis, we provide a thorough characterization of the different in-plane hyperbolic and elliptical PhP modes in GeS. We find not only PhPs with long lifetimes (τ > 2 ps) and excellent THz light confinement (λ0/λ > 45) but also an intrinsic, phonon-induced anomalous dispersion as well as signatures of naturally occurring, substrate-mediated PhP canalization within a single GeS slab.

Nanoscale Valley Modulation by Surface Plasmon Interference.

Excitons in two-dimensional (2D) materials have attracted the attention of the community to develop improved photoelectronic devices. Previous reports are based on direct excitation where the out-of-plane illumination projects a uniform single-mode light spot. However, because of the optical diffraction limit, the minimal spot size is a few micrometers, inhibiting the precise manipulation and control of excitons at the nanoscale level. Herein, we introduced the in-plane coherent surface plasmonic interference (SPI) field to excite and modulate excitons remotely. Compared to the out-of-plane light, a uniform in-plane SPI suggests a more compact spatial volume and an abundance of mode selections for a single or an array of device modulation. Our results not only build up a fundamental platform for operating and encoding the exciton states at the nanoscale level but also provide a new avenue toward all-optical integrated valleytronic chips for future quantum computation and information applications.

Numerical calculation of near-field in vicinity of three-dimensional nano-optical probes using boundary element method.

The diffraction limit is one of the main obstacles in the development of microscopes to analyze the morphology and structure of materials. The main idea of near field scanning optical microscopy (NSOM) is to overcome the diffraction limit using sub-wavelength apertures. In this work, the near-field is simulated in the vicinity of three-dimensional nano-optical apertureless probes. For this purpose, the Helmholtz equation is solved using the boundary element method (BEM). The effects of different parameters on the near field generated in the vicinity of the optical probe are studied. These parameters consist of the length and radius of the probe, the size of the aperture, the angle of the tapered tip, and the geometry of the probe tip. The main advantages of the proposed method are the high accuracy, the very short calculation time, and the ability to calculate the near field inside and outside the optical probe without any approximation.

Numerical Analysis of the Light Modulation by the Frustule of Gomphonema parvulum: The Role of Integrated Optical Components.

Siliceous diatom frustules present a huge variety of shapes and nanometric pore patterns. A better understanding of the light modulation by these frustules is required to determine whether or not they might have photobiological roles besides their possible utilization as building blocks in photonic applications. In this study, we propose a novel approach for analyzing the near-field light modulation by small pennate diatom frustules, utilizing the frustule of Gomphonema parvulum as a model. Numerical analysis was carried out for the wave propagation across selected 2D cross-sections in a statistically representative 3D model for the valve based on the finite element frequency domain method. The influences of light wavelength (vacuum wavelengths from 300 to 800 nm) and refractive index changes, as well as structural parameters, on the light modulation were investigated and compared to theoretical predictions when possible. The results showed complex interference patterns resulting from the overlay of different optical phenomena, which can be explained by the presence of a few integrated optical components in the valve. Moreover, studies on the complete frustule in an aqueous medium allow the discussion of its possible photobiological relevance. Furthermore, our results may enable the simple screening of unstudied pennate frustules for photonic applications.

Nonlinear nanoelectrodynamics of a Weyl metal.

Chiral Weyl fermions with linear energy-momentum dispersion in the bulk accompanied by Fermi-arc states on the surfaces prompt a host of enticing optical effects. While new Weyl semimetal materials keep emerging, the available optical probes are limited. In particular, isolating bulk and surface electrodynamics in Weyl conductors remains a challenge. We devised an approach to the problem based on near-field photocurrent imaging at the nanoscale and applied this technique to a prototypical Weyl semimetal TaIrTe4 As a first step, we visualized nano-photocurrent patterns in real space and demonstrated their connection to bulk nonlinear conductivity tensors through extensive modeling augmented with density functional theory calculations. Notably, our nanoscale probe gives access to not only the in-plane but also the out-of-plane electric fields so that it is feasible to interrogate all allowed nonlinear tensors including those that remained dormant in conventional far-field optics. Surface- and bulk-related nonlinear contributions are distinguished through their "symmetry fingerprints" in the photocurrent maps. Robust photocurrents also appear at mirror-symmetry breaking edges of TaIrTe4 single crystals that we assign to nonlinear conductivity tensors forbidden in the bulk. Nano-photocurrent spectroscopy at the boundary reveals a strong resonance structure absent in the interior of the sample, providing evidence for elusive surface states.

Time-Resolved FDTD and Experimental FTIR Study of Gold Micropatch Arrays for Wavelength-Selective Mid-Infrared Optical Coupling.

Infrared radiation reflection and transmission of a single layer of gold micropatch two-dimensional arrays, of patch length ∼1.0 µm and width ∼0.2 µm, have been carefully studied by a finite-difference time-domain (FDTD) method, and Fourier-transform infrared spectroscopy (FTIR). Through precision design of the micropatch array structure geometry, we achieve a significantly enhanced reflectance (85%), a substantial diffraction (10%), and a much reduced transmittance (5%) for an array of only 15% surface metal coverage. This results in an efficient far-field optical coupling with promising practical implications for efficient mid-infrared photodetectors. Most importantly we find that the propagating electromagnetic fields are transiently concentrated around the gold micropatch array in a time duration of tens of ns, providing us with a novel efficient near-field optical coupling.

Modern Scattering-Type Scanning Near-Field Optical Microscopy for Advanced Material Research.

Infrared and optical spectroscopy represents one of the most informative methods in advanced materials research. As an important branch of modern optical techniques that has blossomed in the past decade, scattering-type scanning near-field optical microscopy (s-SNOM) promises deterministic characterization of optical properties over a broad spectral range at the nanoscale. It allows ultrabroadband optical (0.5-3000 µm) nanoimaging, and nanospectroscopy with fine spatial (<10 nm), spectral (<1 cm-1 ), and temporal (<10 fs) resolution. The history of s-SNOM is briefly introduced and recent advances which broaden the horizons of this technique in novel material research are summarized. In particular, this includes the pioneering efforts to study the nanoscale electrodynamic properties of plasmonic metamaterials, strongly correlated quantum materials, and polaritonic systems at room or cryogenic temperatures. Technical details, theoretical modeling, and new experimental methods are also discussed extensively, aiming to identify clear technology trends and unsolved challenges in this exciting field of research.

Anisotropic Flow Control and Gate Modulation of Hybrid Phonon-Polaritons.

Light-matter interaction in two-dimensional photonic or phononic materials allows for the confinement and manipulation of free-space radiation at sub-wavelength scales. Most notably, the van der Waals heterostructure composed of graphene (G) and hexagonal boron nitride (hBN) provides for gate-tunable hybrid hyperbolic plasmon phonon-polaritons (HP3). Here, we present the anisotropic flow control and gate-voltage modulation of HP3 modes in G-hBN on an air-Au microstructured substrate. Using broadband infrared synchrotron radiation coupled to a scattering-type near-field optical microscope, we launch HP3 waves in both hBN Reststrahlen bands and observe directional propagation across in-plane heterointerfaces created at the air-Au junction. The HP3 hybridization is modulated by varying the gate voltage between graphene and Au. This modifies the coupling of continuum graphene plasmons with the discrete hBN hyperbolic phonon polaritons, which is described by an extended Fano model. This work represents the first demonstration of the control of polariton propagation, introducing a theoretical approach to describe the breaking of the reflection and transmission symmetry for HP3 modes. Our findings augment the degree of control of polaritons in G-hBN and related hyperbolic metamaterial nanostructures, bringing new opportunities for on-chip nano-optics communication and computing.

A mathematical and numerical framework for near-field optics.

This paper is concerned with the inverse problem of reconstructing small and local perturbations of a planar surface using the field interaction between a known plasmonic particle and the planar surface. The aim is to perform a super-resolved reconstruction of these perturbations from shifts in the plasmonic frequencies of the particle-surface system. In order to analyse the interaction between the plasmonic particle and the planar surface, a well-chosen conformal mapping, which transforms the particle-surface system into a coated structure, is used. Then the even Fourier coefficients of the transformed domain are related to the shifts in the plasmonic resonances of the particle-surface system. A direct reconstruction of the perturbations of the planar surface is proposed. Its viability and limitations are documented by numerical examples.

Exploring the Magnetic and Electric Side of Light through Plasmonic Nanocavities.

Light-matter interactions are often considered to be mediated by the electric component of light only, neglecting the magnetic contribution. However, the electromagnetic energy density is equally distributed between both parts of the optical fields. Within this scope, we experimentally demonstrate here, in excellent agreement with numerical simulations, that plasmonic nanostructures can selectively manipulate and tune the magnetic versus electric emission of luminescent nanocrystals. In particular, we show selective enhancement or decay of magnetic and electric emission from trivalent europium-doped nanoparticles in the vicinity of plasmonic nanocavities, designed to efficiently couple to either the electric or magnetic emission of the quantum emitter. Specifically, by precisely controlling the spatial position of the emitter with respect to our plasmonic nanostructures, by means of a near-field optical microscope, we record local distributions of both magnetic and electric radiative local densities of states (LDOS) with nanoscale precision. The distribution of the radiative LDOS reveals the modification of both the magnetic and electric optical quantum environments induced by the presence of the metallic nanocavities. This manipulation and enhancement of magnetic light-matter interaction by means of plasmonic nanostructures opens up new possibilities for the research fields of optoelectronics, chiral optics, nonlinear and nano-optics, spintronics, and metamaterials, among others.

Limits to the Optical Response of Graphene and Two-Dimensional Materials.

Two-dimensional (2D) materials provide a platform for strong light-matter interactions, creating wide-ranging design opportunities via new-material discoveries and new methods for geometrical structuring. We derive general upper bounds to the strength of such light-matter interactions, given only the optical conductivity of the material, including spatial nonlocality, and otherwise independent of shape and configuration. Our material figure-of-merit shows that highly doped graphene is an optimal material at infrared frequencies, whereas single-atomic-layer silver is optimal in the visible. For quantities ranging from absorption and scattering to near-field spontaneous-emission enhancements and radiative heat transfer, we consider canonical geometrical structures and show that in certain cases the bounds can be approached, while in others there may be significant opportunity for design improvement. The bounds can encourage systematic improvements in the design of ultrathin broadband absorbers, 2D antennas, and near-field energy harvesters.

Supercritical angle Raman microscopy: a surface-sensitive nanoscale technique without field enhancement.

Raman scattering microscopy is a versatile tool for label-free imaging and molecular fingerprint analysis. Here, we provide the first demonstration that the selective collection of scattered signals exceeding the critical angle for total internal reflection enables surface-confined spontaneous Raman investigations at nanometre resolution. This high-axial selectivity leads to improved signal-to-background ratios, thus making this technique an excellent probe for surface-related molecular specimens. The richness of the spectroscopic information obtained through the supercritical angle Raman (SAR) collection path was proven by comparing its output with that of a parallel far-field collection path. Furthermore, we demonstrated that the proposed SAR technique is a versatile microscopy approach that can be used alone or in combination with amplified Raman modalities such as surface-enhanced resonance Raman scattering.

Plasmonic Structures, Materials and Lenses for Optical Lithography beyond the Diffraction Limit: A Review.

The rapid development of nanotechnologies and sciences has led to the great demand for novel lithography methods allowing large area, low cost and high resolution nano fabrications. Characterized by unique sub-diffraction optical features like propagation with an ultra-short wavelength and great field enhancement in subwavelength regions, surface plasmon polaritons (SPPs), including surface plasmon waves, bulk plasmon polaritons (BPPs) and localized surface plasmons (LSPs), have become potentially promising candidates for nano lithography. In this paper, investigations into plasmonic lithography in the manner of point-to-point writing, interference and imaging were reviewed in detail. Theoretical simulations and experiments have demonstrated plasmonic lithography resolution far beyond the conventional diffraction limit, even with ultraviolet light sources and single exposure performances. Half-pitch resolution as high as 22 nm (~1/17 light wavelength) was observed in plasmonic lens imaging lithography. Moreover, not only the overview of state-of-the-art results, but also the physics behind them and future research suggestions are discussed as well.

Stacking Structures of Few-Layer Graphene Revealed by Phase-Sensitive Infrared Nanoscopy.

The stacking orders in few-layer graphene (FLG) strongly influences the electronic properties of the material. To explore the stacking-specific properties of FLG in detail, one needs powerful microscopy techniques that visualize stacking domains with sufficient spatial resolution. We demonstrate that infrared (IR) scattering scanning near-field optical microscopy (sSNOM) directly maps out the stacking domains of FLG with a nanometric resolution, based on the stacking-specific IR conductivities of FLG. The intensity and phase contrasts of sSNOM are compared with the sSNOM contrast model, which is based on the dipolar tip-sample coupling and the theoretical conductivity spectra of FLG, allowing a clear assignment of each FLG domain as Bernal, rhombohedral, or intermediate stacks for tri-, tetra-, and pentalayer graphene. The method offers 10-100 times better spatial resolution than the far-field Raman and infrared spectroscopic methods, yet it allows far more experimental flexibility than the scanning tunneling microscopy and electron microscopy.

Near-field microscopy with a scanning nitrogen-vacancy color center in a diamond nanocrystal: A brief review.

We review our recent developments of near-field scanning optical microscopy (NSOM) that uses an active tip made of a single fluorescent nanodiamond (ND) grafted onto the apex of a substrate fiber tip. The ND hosting a limited number of nitrogen-vacancy (NV) color centers, such a tip is a scanning quantum source of light. The method for preparing the ND-based tips and their basic properties are summarized. Then we discuss theoretically the concept of spatial resolution that is achievable in this special NSOM configuration and find it to be only limited by the scan height over the imaged system, in contrast with the standard aperture-tip NSOM whose resolution depends critically on both the scan height and aperture diameter. Finally, we describe a scheme we have introduced recently for high-resolution imaging of nanoplasmonic structures with ND-based tips that is capable of approaching the ultimate resolution anticipated by theory.

Origin and Future of Plasmonic Optical Tweezers.

Plasmonic optical tweezers can overcome the diffraction limits of conventional optical tweezers and enable the trapping of nanoscale objects. Extension of the trapping and manipulation of nanoscale objects with nanometer position precision opens up unprecedented opportunities for applications in the fields of biology, chemistry and statistical and atomic physics. Potential applications include direct molecular manipulation, lab-on-a-chip applications for viruses and vesicles and the study of nanoscale transport. This paper reviews the recent research progress and development bottlenecks and provides an overview of possible future directions in this field.

Spectral and mode properties of surface plasmon polariton waveguides studied by near-field excitation and leakage-mode radiation measurement.

We present a method to couple surface plasmon polariton (SPP) guiding mode into dielectric-loaded SPP waveguide (DLSPPW) devices with spectral and mode selectivity. The method combined a transmission-mode near-field spectroscopy to excite the SPP mode and a leakage radiation optical microscope for direct visualization. By using a near-field fiber tip, incident photons with different wavelengths were converted into SPPs at the metal/dielectric interface. Real-time SPP radiation images were taken through leakage radiation images. The wavelength-dependent propagation lengths for silver- and gold-based DLSPPWs were measured and compared. It confirms that silver-based SPP has a propagation length longer than a gold-based one by 1.25, 1.38, and 1.52 times for red, green, and blue photons. The resonant coupling as a function of wavelength in dual DLSPPWs was measured. The coupling lengths measured from leakage radiation images were in good agreement with finite-difference time domain simulations. In addition, the propagation profile due to multi-SPP modes interference was studied by changing position of the fiber tip. In a multimode DLSPPW, SPP was split into two branches with a gap of 2.237 µm when the tip was at the center of the waveguide. It became a zigzag profile when the SPP was excited at the corner of the waveguide.