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This Article describes a method for the characterization of the imaging performance of tip-enhanced Raman spectroscopy probes. The proposed method identifies single-walled carbon nanotubes that are suitable as one-dimensional Raman scattering objects by using atomic force microscope maps and exciting the radial breathing mode using 785 nm illumination. High-resolution cross sections of the nanotubes are collected, and the point spread functions are calculated along with the optical contrast and spot diameter. The method is used to characterize several probes, which results in a set of imaging recommendations and a summary of limitations for each probe. Elemental analysis and boundary element simulations are used to explain the formation of multiple peaks in the point spread functions as a consequence of random grain formation on the probe surface. [ABSTRACT FROM AUTHOR]

Terahertz (THz) technology holds great potential across diverse applications, including biosensing and information communications, but conventional far-field techniques are limited by diffraction. Near-field optical microscopy overcomes this barrier through a sharp tip that concentrates incident THz waves into nanometric volumes, detecting scattered near-field to reveal nanoscale optical properties. However, owing to the large THz wavelengths, resonant surface waves arising on the tip and cantilever obscure the intrinsic response. Here we combine near-field microscopy with THz time-domain spectroscopy and implement time-domain filtering with an elongated cantilever to eliminate this artifact, achieving intrinsic nanospectroscopy and nanoimaging. By applying this technique, we distinguish and characterize historical pigments of an ancient sculpture, such as vermilion and red lead, on the nanoscale. We also unravel deep-subwavelength localized resonance modes in THz optical antennas, demonstrating capabilities for THz nanophotonics. Our work advances THz nanoimaging and nanospectroscopy techniques to probe intrinsic nanoscale THz light-matter interactions.

Plasmonic metasurfaces with spatial symmetry breaking are crucial materials with significant applications in fields such as polarization-controlled photonic devices and nanophotonic platforms for chiral sensing. In this paper, we introduce planar plasmonic metasurfaces, less than one-tenth of a wavelength thick, featuring nanocavities formed by three equilateral triangles. This configuration creates uniform, thin metasurfaces. Through a combination of experimental measurements and numerical modeling, we demonstrate the inherent superchirality of these plasmonic metasurfaces. We address the challenge of achieving a strong enhancement of optical chirality in the visible spectrum, reaching levels comparable to those of 3D chiral metasurfaces.

Observation of interlayer, charge transfer (CT) excitons in van der Waals heterostructures (vdWHs) based on 2D-2D systems has been well investigated. While conceptually interesting, these charge transfer excitons are highly delocalized and spatially localizing them requires twisting layers at very specific angles. This issue of localizing the CT excitons can be overcome via making nanoplate-2D material heterostructures (N2DHs) where one of the components is a spatially quantum confined medium. Here, we demonstrate the formation of CT excitons in a mixed dimensional system comprising MoSe 2 and WSe 2 monolayers and CdSe/CdS-based core/shell nanoplates (NPLs). Spectral signatures of CT excitons in our N2DHs were resolved locally at the 2D/single-NPL heterointerface using tip-enhanced photoluminescence (TEPL) at room temperature. By varying both the 2D material and the shell thickness of the NPLs and applying an out-of-plane electric field, the exciton resonance energy was tuned by up to 100 meV. Our finding is a significant step toward the realization of highly tunable N2DH-based next-generation photonic devices.

Coupling effects of localized surface plasmon resonance (LSPR) represent an efficient means to tune the plasmonic modes and to enhance the near-field. While LSPR coupling in metal nanoparticles has been extensively explored, limited attention has been given to heavily doped semiconductor nanocrystals. Here, we investigate the LSPR coupling behavior of Cs-doped tungsten oxide (Cs x WO 3-δ ) nanocrystal platelets as they undergo an oriented assembly into parallel stacks. The oriented assembly was achieved by lowering the dispersion stability of the colloidal nanoplatelets, of which the basal surface was selectively ligand-functionalized. This assembly induces simultaneous blue-shifts and red-shifts of dual-mode LSPR peaks without compromising the intensity and quality factor. This stands in contrast to the significant damping, broadening, and overall red-shift of the LSPR observed in random assemblies. Computational simulations successfully replicate the experimental observations, affirming the potential of this coupling phenomenon of near-infrared dual-mode LSPR in diverse applications including solar energy, bio-optics, imaging, and telecommunications.

Here, we describe the synthesis of a plasmonic particle-in-a-frame architecture in which a solid Au octahedron is enclosed by a Au cubic nanoframe. The octahedra are positioned inside and surrounded by outer Au cubic nanoframes, creating intra-nanogaps within a single entity. Six sharp vertexes in the Au octahedra point toward the open (100) facets of the cubic nanoframes. This allows not only efficient interactions with the surroundings but also tip-enhanced electromagnetic near-field focusing at the sharp tips of the octahedra, combined with intraparticle coupling. The solid core-frame shell structure enhances near-field focusing, giving rise to a heightened concentration of "hot spots". This effect enables highly sensitive detection of 2-naphthalenethiol and thiram, indicating these substrates for use in surface-enhanced Raman spectroscopy-related applications.

Waveguides play a key role in the implementation of on-chip optical elements and, therefore, lie at the heart of integrated photonics. To add the functionalities of layered materials to existing technologies, dedicated fabrication protocols are required. Here, we build on laser writing to pattern grating structures into bulk noncentrosymmetric transition metal dichalcogenides with grooves as sharp as 250 nm. Using thin flakes of 3R-MoS 2 that act as waveguides for near-infrared light, we demonstrate the functionality of the grating couplers with two complementary experiments: first, nano-optical imaging is used to visualize transverse electric and magnetic modes, whose directional outcoupling is captured by finite element simulations. Second, waveguide second-harmonic generation is demonstrated by grating-coupling femtosecond pulses into the slabs in which the radiation partially undergoes frequency doubling throughout the propagation. Our work provides a straightforward strategy for laser patterning of van der Waals crystals, demonstrates the feasibility of compact frequency converters, and examines the tuning knobs that enable optimized coupling into layered waveguides.

Herein, we present a synthetic approach to fabricate Au nanoheptamers composed of six individual Au nanospheres interconnected through thin metal bridges arranged in an octahedral configuration. The resulting structures envelop central Au nanospheres, producing Au nanosphere heptamers with an open architectural arrangement. Importantly, the initial Pt coating of the Au nanospheres is a crucial step for protecting the inner Au nanospheres during multiple reactions. As-synthesized Au nanoheptamers exhibit multiple hot spots formed by nanogaps between nanospheres, resulting in strong electromagnetic near-fields. Additionally, we conducted surface-enhanced Raman-scattering-based detection of a chemical warfare agent simulant in the gas phase and achieved a limit of detection of 100 ppb, which is 3 orders lower than that achieved using Au nanospheres and Au nanohexamers. This pseudocore-shell nanostructure represents a significant advancement in the realm of complex nanoparticle synthesis, moving the field one step closer to sophisticated nanoparticle engineering.

We perform scanning microwave microscopy (SMM) to study the spatially varying electronic properties and related morphology of pristine and degraded methylammonium lead-halide (MAPI) perovskite films fabricated under different ambient humidity. We find that higher processing humidity leads to the emergence of increased conductivity at the grain boundaries but also correlates with the appearance of resistive grains that contain PbI2. Deteriorated films show larger and increasingly insulating grain boundaries as well as spatially localized regions of reduced conductivity within grains. These results suggest that while humidity during film fabrication primarily benefits device properties due to the passivation of traps at the grain boundaries and self-doping, it also results in the emergence of PbI2-containing grains. We further establish that MAPI film deterioration under ambient conditions proceeds via the spatially localized breakdown of film conductivity, both at grain boundaries and within grains, due to local variations in susceptibility to deterioration. These results confirm that PbI2 has both beneficial and adverse effects on device performance and provide new means for device optimization by revealing spatial variations in sample conductivity as well as morphological differences in resistance to sample deterioration. [ABSTRACT FROM AUTHOR]

Key requirements for quantum plasmonic nanocircuits are reliable single-photon sources, high coupling efficiency to the plasmonic structures, and low propagation losses. Self-assembled epitaxially grown GaAs quantum dots are close to ideal as stable, bright, and narrowband single-photon emitters. Likewise, wet-chemically grown monocrystalline silver nanowires are among the best plasmonic waveguides. However, large propagation losses of surface plasmons on the high-index GaAs substrate prevent their direct combination. Here, we show by experiment and simulation that the best overall performance of the quantum plasmonic nanocircuit based on these building blocks is achieved in the intermediate field regime with an additional spacer layer between the quantum dot and the plasmonic waveguide. High-resolution cathodoluminescence measurements allow a precise determination of the coupling distance and support a simple analytical model to explain the overall performance. The coupling efficiency is increased up to four times by standing wave interference near the end of the waveguide.

A synthesis method for plasmonic double-walled nanoframes was developed, where single-walled truncated octahedral nanoframes with (111) open facets and (100) solid flat planes are nested in a core-shell manner. By applying multiple chemical toolkits to Au cuboctahedrons as a starting template, Au double-walled nanoframes with controllable face-to-face nanogaps were successfully synthesized in high homogeneity in size and shape. Importantly, when the gap distance between inner and outer flat walled frames became closer, augmentation of electromagnetic near-field focusing was achieved, leading to generation of hot-zones, which was verified by surface-enhanced Raman spectroscopy. The unique optical property of Au double-walled nanoframes with high structural intricacy was carefully investigated and the SERS substrates comprising Au double-walled nanoframes with the narrowest nanogaps exhibited much improved near-field enhancement toward strongly and/or weakly adsorbing analytes, allowing for gas phase detection in chemical warfare agents, which is a huge challenge in early warning systems.

Nanocavities formed by ultrathin metallic gaps permit the reproducible engineering and enhancement of light-matter interaction, with mode volumes reaching the smallest values allowed by quantum mechanics. While the enhanced vacuum field in metallic nanogaps has been firmly evidenced, fewer experimental reports have examined the far-field to near-field input coupling under strongly focused laser beam. Here, we experimentally demonstrate selective excitation of nanocavity modes controlled by the polarization and frequency of the laser beam. We reveal mode selectivity by recording confocal maps of Raman scattering excited by cylindrical vector beams, which are compared to the known excitation near-field patterns. Our measurements reveal the transverse vs longitudinal polarization of the excited antenna mode and how the input coupling rate depends on laser wavelength. The method introduced here is easily applicable to other experimental scenarios, and our results help connect far-field with near-field parameters in quantitative models of nanocavity-enhanced phenomena.

Graphene nano-optics at terahertz (THz) frequencies (ν) is theoretically anticipated to feature extraordinary effects. However, interrogating such phenomena is nontrivial, since the atomically thin graphene dimensionally mismatches the THz radiation wavelength reaching hundreds of micrometers. Greater challenges happen in the THz gap (0.1-10 THz) wherein light sources are scarce. To surpass these barriers, we use a nanoscope illuminated by a highly brilliant and tunable free-electron laser to image the graphene nano-optical response from 1.5 to 6.0 THz. For ν < 2 THz, we observe a metal-like behavior of graphene, which screens optical fields akin to noble metals, since this excitation range approaches its charge relaxation frequency. At 3.8 THz, plasmonic resonances cause a field-enhancement effect (FEE) that improves the graphene imaging power. Moreover, we show that the metallic behavior and the FEE are tunable upon electrical doping, thus providing further control of these graphene nano-optical properties in the THz gap.

Long regarded as a model system for studying insulator-to-metal phase transitions, the correlated electron material vanadium dioxide (VO2) is now finding novel uses in device applications. Two of its most appealing aspects are its accessible transition temperature (~341 K) and its rich phase diagram. Strain can be used to selectively stabilize different VO2 insulating phases by tuning the competition between electron and lattice degrees of freedom. It can even break the mesoscopic spatial symmetry of the transition, leading to a quasiperiodic ordering of insulating and metallic nanodomains. Nanostructuring of strained VO2 could potentially yield unique components for future devices. However, the most spectacular property of VO2--its ultrafast transition--has not yet been studied on the length scale of its phase heterogeneity. Here, we use ultrafast near-field microscopy in the mid-infrared to study individual, strained VO2 nanobeams on the 10 nm scale. We reveal a previously unseen correlation between the local steady-state switching susceptibility and the local ultrafast response to below-threshold photoexcitation. These results suggest that it may be possible to tailor the local photoresponse of VO2 using strain and thereby realize new types of ultrafast nano-optical devices. [ABSTRACT FROM AUTHOR]

Using an efficient implementation of the discrete dipole approximation and topology optimization, we design all-dielectric metasurfaces capable of focusing light into intense deep subwavelength hotspots. The light focusing of these metasurfaces far outweighs conventional lenses and can provide dramatic enhancements of processes that depend superlinearly on light intensity, such as light-powered membrane distillation and photocatalysis. Our approach can easily be generalized to optimize metasurfaces for other functionalities, such as nonlinear optics or photothermal conversion.

We measure near-field radiative cooling of a thermally isolated nanostructure up to a few degrees and show that in principle this process can efficiently cool down localized hotspots by tens of degrees at submicrometer gaps. This process of cooling is achieved without any physical contact, in contrast to heat transfer through conduction, thus enabling novel cooling capabilities. We show that the measured trend of radiative cooling agrees well theoretical predictions and is limited mainly by the geometry of the probe used here as well as the minimum separation that could be achieved in our setup. These results also pave the way for realizing other new effects based on resonant heat transfer, like thermal rectification and negative thermal conductance. [ABSTRACT FROM AUTHOR]

Ultrastrong coupling of light and matter creates new opportunities to modify chemical reactions or develop novel nanoscale devices. One-dimensional Luttinger-liquid plasmons in metallic carbon nanotubes are long-lived excitations with extreme electromagnetic field confinement. They are promising candidates to realize strong or even ultrastrong coupling at infrared frequencies. We applied near-field polariton interferometry to examine the interaction between propagating Luttinger-liquid plasmons in individual carbon nanotubes and surface phonon polaritons of silica and hexagonal boron nitride. We extracted the dispersion relation of the hybrid Luttinger-liquid plasmon-phonon polaritons (LPPhPs) and explained the observed phenomena by the coupled harmonic oscillator model. The dispersion shows pronounced mode splitting, and the obtained value for the normalized coupling strength shows we reached the ultrastrong coupling regime with both native silica and hBN phonons. Our findings predict future applications to exploit the extraordinary properties of carbon nanotube plasmons, ranging from nanoscale plasmonic circuits to ultrasensitive molecular sensing.

Plasmonic self-assembled nanocavities are ideal platforms for extreme light localization as they deliver mode volumes of <50 nm 3 . Here we show that high-order plasmonic modes within additional micrometer-scale resonators surrounding each nanocavity can boost light localization to intensity enhancements >10 5 . Plasmon interference in these hybrid microresonator nanocavities produces surface-enhanced Raman scattering (SERS) signals many-fold larger than in the bare plasmonic constructs. These now allow remote access to molecules inside the ultrathin gaps, avoiding direct irradiation and thus preventing molecular damage. Combining subnanometer gaps with micrometer-scale resonators places a high computational demand on simulations, so a generalized boundary element method (BEM) solver is developed which requires 100-fold less computational resources to characterize these systems. Our results on extreme near-field enhancement open new potential for single-molecule photonic circuits, mid-infrared detectors, and remote spectroscopy.

Coupling between plasmonic nanoparticles (NPs) in nanoparticle assemblies has been investigated extensively via far-field properties, such as absorption and scattering, but very rarely via near-field properties, and a quantitative investigation of near-field properties should provide great insight into the nature of the coupling. We report a numerical procedure to obtain reliable near-field spectra ( Q NF ) around spherical gold nanoparticles (Au NPs) using Discrete Dipole Approximation (DDA). The reliability of the method was tested by comparing Q NF from DDA calculations with exact results from the Mie theory. We then applied the method to examine Au NPs assembled in dimer, trimer, and up to pentamer in a linear arrangement. For the well-studied dimer system, we show that the Q NF enhancement, due to coupling in longitudinal mode, is much greater than the enhancement in Q ext . There is a linear correlation between the Q NF and Q ext peak positions, with the Q NF peak redshifted from the Q ext peak by an average of approximately 12 nm. In the case of the multimers, Q NF spectra from individual spheres were not always identical and become dependent on the sphere location. In the longitudinal model, the center sphere has the strongest Q NF spectra. For the transverse mode, we differentiate two different scenario, transverse-Y where both electric field ( E ) and light propagation vector ( k ) are perpendicular the chain axis, and transverse-X where k is parallel to the chain axis. In transverse-Y mode, coupling leads to reduced Q NF spectra and the center sphere has the lowest Q NF intensity. In transverse-X mode, there is retardation effect from the front sphere to the back sphere. The Q NF from the front sphere is stronger than from the back sphere. In addition, due to the phase lag in k -direction, the Q NF in transverse-X can differ quite significantly from transverse-Y for large particles. All these results could be understood when one considers how electric field from induced dipoles on neighboring NPs add on or subtract from the incident E-field. These results provide new insight into the coupling properties of Au NPs.

The conventional notion for achieving high efficiency in thermophotovoltaics (TPVs) is to use a monochromatic emission at a photon energy corresponding to the band gap of the cell. Here, we prove theoretically that such a notion is only accurate under idealized conditions and further show that, when nonradiative recombination is taken into account, efficiency improvement can be achieved by broadening the emission spectrum, due to an enhancement in the open-circuit voltage. Broadening the emission spectrum also improves the electrical power density, by increasing the short-circuit current. Hence, broadening the emission spectrum can simultaneously improve the efficiency and power density of practical TPV systems. To illustrate these findings, we focus on surface polariton-mediated near-field TPVs. We propose a versatile design strategy for broadening the emission spectrum via stacking of multiple plasmonic thin film layers. As an example, we consider a realistic ITO/InAs TPV and predict a conversion efficiency of 50% simultaneously with a power density of nearly 80 W/cm 2 at a 1300 K emitter temperature. The performance of our proposed system far exceeds previous works in similar systems using a single plasmonic layer emitter.

Phonon-polaritons (PhPs) in layered crystals, including hexagonal boron nitride (hBN), have been investigated by combined scattering-type scanning near-field optical microscopy (s-SNOM) and Fourier transform infrared (FTIR) spectroscopy. Nevertheless, many of such s-SNOM-based FTIR spectra features remain unexplored, especially those originated from the impact of boundaries. Here we observe real-space PhP propagations in thin-layer hBN sheets either supported or suspended by s-SNOM imaging. Then with a high-power broadband IR laser source, we identify two major peaks and multiple auxiliary peaks in the near-field amplitude spectra, obtained using scattering-type near-field FTIR spectroscopy, from both supported and suspended hBN. The major PhP propagation interference peak moves toward the major in-plane phonon peak when the IR illumination moves away from the hBN edge. Specific differences between the auxiliary peaks in the near-field amplitude spectra from supported and suspended hBN sheets are investigated regarding different boundary conditions, associated with edges and substrate interfaces. The outcomes may be explored in heterostructures for advanced nanophotonic applications.

We present a new methodology that enables studies of the molecular structure of graphene-liquid interfaces with nanoscale spatial resolution. It is based on Fourier transform infrared nanospectroscopy (nano-FTIR), where the infrared (IR) field is plasmonically enhanced near the tip apex of an atomic force microscope (AFM). The graphene seals a liquid electrolyte reservoir while acting also as a working electrode. The photon transparency of graphene enables IR spectroscopy studies of its interface with liquids, including water, propylene carbonate, and aqueous ammonium sulfate electrolyte solutions. We illustrate the method by comparing IR spectra obtained by nano-FTIR and attenuated total reflection (which has a detection depth of a few microns) demonstrating that the nano-FTIR method makes it possible to determine changes in speciation and ion concentration in the electric double and diffuse layers as a function of bias.

Thermal radiation transfer between two objects separated by a subwavelength gap (near-field thermal radiation transfer) can be orders of magnitude larger than that in free space, which is attracting increasing attention with respect to both fundamental nanoscience and its potential for high-power-density and high-efficiency conversion of heat to electricity in thermophotovoltaic (TPV) systems. However, the realization of near-field thermal radiation transfer in TPV systems involves significant challenges because it requires a subwavelength gap and large temperature difference between the emitter and the PV cell while minimizing the heat transfer that does not contribute to the photocurrent generation. To overcome these challenges, here we demonstrate a one-chip near-field TPV device consisting of a thin-film Si emitter and InGaAs PV cell with an intermediate Si substrate, which enables the suppression of the heat transfer due to sub-bandgap radiation by free carriers and surface modes. Through the one-chip integration and thermal isolation using Si process technologies, we realize a deep subwavelength gap (<150 nm) between the emitter and the intermediate substrate without using any external positioners while maintaining a large temperature difference (>700 K). Compared to the equivalent device operating in the far-field regime, we achieve 10-fold enhancement of the photocurrent in the PV cell without degrading the open-circuit voltage and fill factor, demonstrating the potential of our one-chip device for the future applications of near-field thermal radiation transfer.

We report systematic design and formation of plasmonic perovskite solar cells (PSCs) by integrating Au@TiO 2 core-shell nanoparticles (NPs) into porous TiO 2 and/or perovskite semiconductor capping layers. The plasmonic effects in the formed PSCs are examined. The most efficient configuration is obtained by incorporating Au@TiO 2 NPs into both the porous TiO 2 and the perovskite capping layers, which increases the power conversion efficiency (PCE) from 12.59% to 18.24%, demonstrating over 44% enhancement, compared with the reference device without the metal NPs. The PCE enhancement is mainly attributed to short-circuit current improvement. The plasmonic enhancement effects of Au@TiO 2 core-shell nanosphere photovoltaic composites are explored based on the combination of UV-vis absorption spectroscopy, external quantum efficiency (EQE), photocurrent properties, and photoluminescence (PL). The addition of Au@TiO 2 nanospheres increased the rate of exciton generation and the probability of exciton dissociation, enhancing charge separation/transfer, reducing the recombination rate, and facilitating carrier transport in the device. This study contributes to understanding of plasmonic effects in perovskite solar cells and also provides a promising approach for simultaneous photon energy and electron management.

Phase separations in ternary/multinary semiconductor alloys is a major challenge that limits optical and electronic internal device efficiency. We have found ubiquitous local phase separation in In1-xGaxN alloys that persists to nanoscale spatial extent by employing high-resolution nanoimaging technique. We lithographically patterned InN/sapphire substrates with nanolayers of In1-xGaxN down to few atomic layers thick that enabled us to calibrate the near-field infrared response of the semiconductor nanolayers as a function of composition and thickness. We also developed an advanced theoretical approach that considers the full geometry of the probe tip and all the sample and substrate layers. Combining experiment and theory, we identified and quantified phase separation in epitaxially grown individual nanoalloys. We found that the scale of the phase separation varies widely from particle to particle ranging from all Ga- to all In-rich regions and covering everything in between. We have found that between 20 and 25% of particles show some level of Ga-rich phase separation over the entire sample region, which is in qualitative agreement with the known phase diagram of In1-xGaxN system.

We demonstrate a far-field single molecule super-resolution method that maps plasmonic near-fields. The method is largely invariant to fluorescence quenching (arising from probe proximity to a metal), has reduced point-spread-function distortion compared to fluorescent dyes (arising from strong coupling to nanoscopic metallic features), and has a large dynamic range (of 2 orders of magnitude) allowing mapping of plasmonic field-enhancements regions. The method takes advantage of the sensitivity of quantum dot (QD) stochastic blinking to plasmonic near-fields. The modulation of the blinking characteristics thus provides an indirect measure of the local field strength. Since QD blinking can be monitored in the far-field, the method can measure localized plasmonic near-fields at high throughput using a simple far-field optical setup. Using this method, propagation lengths and penetration depths were mapped-out for silver nanowires of different diameters and for different dielectric environments, with a spatial accuracy of ∼15 nm. We initially use sparse sampling to ensure single molecule localization for accurate characterization of the plasmonic near-field with plans to increase density of emitters in further studies. The measured propagation lengths and penetration depths values agree well with Maxwell finite-difference time-domain calculations and with published literature values. This method offers advantages such as low cost, high throughput, and superresolved mapping of localized plasmonic fields at high sensitivity and fidelity.

Fabrication of large-area, highly orderly, and high-resolution nanostructures in a cost-effective fashion prompts advances in nanotechnology. Herein, for the first time, we demonstrate a unique strategy to prepare a long-range highly regular polymer lens from photoresist nanotrenches based templates, which are obtained from underexposure. The relationship between exposure dose and the cross-sectional morphology of produced photoresist nanostructures is revealed for the first time. The polymer lens arrays are repeatedly used for rapid generation of sub-100 nm nanopatterns across centimeter-scale areas. The light focusing properties of the nanoscale polymer lens are investigated by both simulation and experiment. It is found that the geometry, size of the lens, and the exposure dose can be deployed to adjust the produced feature size, spacing, and shapes. Because the polymer lenses are derived from top-down photolithography, the nearly perfect long-range periodicity of produced nanopatterns is ensured, and the feature shapes can be flexibly designed. Because this nanolithographic strategy enables subwavelength periodical nanopatterns with controllable feature size, geometry, and composition in a cost-effective manner, it can be optimized as a viable and potent nanofabrication tool for various technological applications.

Laser processing with optically trapped microspheres is a promising tool for nanopatterning at subdiffraction-limited resolution in a wide range of technological and biomedical applications. In this paper, we investigate subdiffraction-limited structuring of borosilicate glass with femtosecond pulses in the near-field of optically trapped microspheres combined with chemical postprocessing. The glass surface was processed by single laser pulses at 780 nm focused by silica microspheres and then subjected to selective etching in KOH, which produced pits in the laser-affected zones (LAZs). Chemical postprocessing allowed obtaining structures with better resolution and reproducibility. We demonstrate production of reproducible pits with diameters as small as 70 nm (λ/11). Complex two-dimensional structures with 100 nm (λ/8) resolution were written on the glass surface point by point with microspheres manipulated by optical tweezers. Furthermore, the mechanism of laser modification underlying selective etching was investigated with mass spectrum analysis. We propose that the increased etching rate of laser-treated glass results from changes in its chemical composition and oxygen deficiency.

Scattering scanning near-field optical microscopy (s-SNOM) has emerged as a powerful nanoscale spectroscopic tool capable of characterizing individual biomacromolecules and molecular materials. However, applications of scattering-based near-field techniques in the infrared (IR) to native biosystems still await a solution of how to implement the required aqueous environment. In this work, we demonstrate an IR-compatible liquid cell architecture that enables near-field imaging and nanospectroscopy by taking advantage of the unique properties of graphene. Large-area graphene acts as an impermeable monolayer barrier that allows for nano-IR inspection of underlying molecular materials in liquid. Here, we use s-SNOM to investigate the tobacco mosaic virus (TMV) in water underneath graphene. We resolve individual virus particles and register the amide I and II bands of TMV at ca. 1520 and 1660 cm(-1), respectively, using nanoscale Fourier transform infrared spectroscopy (nano-FTIR). We verify the presence of water in the graphene liquid cell by identifying a spectral feature associated with water absorption at 1610 cm(-1).

A reproducible route for tuning localized surface plasmon resonance in scattering type near-field optical microscopy probes is presented. The method is based on the production of a focused-ion-beam milled single groove near the apex of electrochemically etched gold tips. Electron energy-loss spectroscopy and scanning transmission electron microscopy are employed to obtain highly spatially and spectroscopically resolved maps of the milled probes, revealing localized surface plasmon resonance at visible and near-infrared wavelengths. By changing the distance L between the groove and the probe apex, the localized surface plasmon resonance energy can be fine-tuned at a desired absorption channel. Tip-enhanced Raman spectroscopy is applied as a test platform, and the results prove the reliability of the method to produce efficient scattering type near-field optical microscopy probes.

Optimizing new generations of two-dimensional devices based on van der Waals materials will require techniques capable of measuring variations in electronic properties in situ and with nanometer spatial resolution. We perform scanning microwave microscopy (SMM) imaging of single layers of MoS2 and n- and p-doped WSe2. By controlling the sample charge carrier concentration through the applied tip bias, we are able to reversibly control and optimize the SMM contrast to image variations in electronic structure and the localized effects of surface contaminants. By further performing tip bias-dependent point spectroscopy together with finite element simulations, we distinguish the effects of the quantum capacitance and determine the local dominant charge carrier species and dopant concentration. These results underscore the capability of SMM for the study of 2D materials to image, identify, and study electronic defects.

With the development of nanoscience and nanotechnology for the bottom-up nanofabrication of nanostructures formed from polystyrene nanoparticles, joining technology is an essential step in the manufacturing and assembly of nanodevices and nanostructures in order to provide mechanical integration and connection. To study the nanospot welding of polystyrene nanoparticles, we propose a new nanospot-soldering method using the near-field enhancement effect of a metallic atomic force microscope (AFM) probe tip that is irradiated by an optical fiber probe laser. On the basis of our theoretical analysis of the near-field enhancement effect, we set up an experimental system for nanospot soldering; this approach is carried out by using an optical fiber probe laser to irradiate the AFM probe tip to sinter the nanoparticles, providing a promising technical approach for the application of nanosoldering in nanoscience and nanotechnology.

Boron nitride (BN) is considered to be a promising substrate for graphene-based devices in part because its large band gap can serve to insulate graphene in layered heterostructures. At mid-infrared frequencies, graphene supports surface plasmon polaritons (SPPs), whereas hexagonal-BN (h-BN) is found to support surface phonon polaritons (SPhPs). We report on the observation of infrared polaritonic coupling between graphene SPPs and boron nitride nanotube (BNNT) SPhPs. Infrared scattering type scanning near-field optical microscopy is used to obtain spatial distribution of the two types of polaritons at the nanoscale. The observation suggests that those polaritons interact at the nanoscale in a one-dimensional/two-dimensional (1D/2D) geometry, exchanging energy in a nonplanar configuration at the nanoscale. Control of the polaritonic interaction is achieved by adjustment of the graphene Fermi level through voltage gating. Our observation suggests that boron nitride nanotubes and graphene can interact at mid-infrared frequencies and coherently exchange their energies at the nanoscale through the overlap of mutual electric near field of surface phonon polaritons and surface plasmon polaritons. Such interaction enables the design of nano-optical devices based on BNNT-graphene polaritonics in the mid-infrared range.

Polarization analysis in tip-enhanced Raman spectroscopy (TERS) is of tremendous advantage, as it allows one to study highly directional intrinsic properties of a sample at the nanoscale. However, neither evaluation nor control of the polarization properties of near-field light in TERS is as straightforward as in usual far-field illumination, because of the random metallic nanostructure attached to the tip apex. In this study, we have developed a method to successfully analyze the polarization of near-field light in TERS from the scattering pattern produced by the induced dipole in the metallic tip. Under dipole approximation, we measured the image of the dipole at a plane away from the focal plane, where the information about the direction of the dipole oscillation was intact. The direction of the dipole oscillation was determined from the defocused pattern, and then the polarization of near-field light was evaluated from the oscillation direction by calculating the intensity distribution of near-field light through Green's function. After evaluating the polarization of some fabricated tips, we used those tips to measure TERS images from single-walled carbon nanotubes and confirmed that the contrast of the TERS image depended on the oscillation direction of the dipole, which were also found in excellent agreement with the calculated TERS images, verifying that the polarization of the near-field was quantitatively estimated by our technique. Our technique would lead to better quantitative analysis in TERS imaging with consideration of polarization impact, giving a better understanding of the behavior of nanomaterials.

We present a direct measurement of short-wavelength plasmons focused into a sub-100 nm spot in homogeneous (translation invariant) 2D space. The short-wavelength (SW) surface plasmon polaritons (SPP) are achieved in metal-insulator-insulator (MII) platform consisting of silver, silicon nitride, and air. This platform is homogeneous in two spatial directions and supports SPP at wavelength more than two times shorter than that in free space yet interacts with the outer world through the evanescent tail in air. We use an apertureless (scattering) near-field scanning optical microscope (NSOM) to map directly the amplitude and phase of these SW-SPP and show they can be focused to under 70 nm without structurally assisted confinement such as nanoantennas or nanofocusing. This, along with the use of visible light at 532 nm which is suitable for optical microscopy, can open new directions in direct biological and medical imaging at the sub-100 nm resolution regime.