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.

Editorial for the Special Issue on Tunable Nanophotonics and Reconfigurable Metadevices.

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All-Optical Reconfigurable Excitonic Charge States in Monolayer MoS2.

Excitons are quasi-particles composed of electron-hole pairs through Coulomb interaction. Due to the atomic-thin thickness, they are tightly bound in monolayer transition metal dichalcogenides (TMDs) and dominate their optical properties. The capability to manipulate the excitonic behavior can significantly influence the photon emission or carrier transport performance of TMD-based devices. However, on-demand and region-selective manipulation of the excitonic states in a reversible manner remains challenging so far. Herein, harnessing the coordinated effect of femtosecond-laser-driven atomic defect generation, interfacial electron transfer, and surface molecular desorption/adsorption, we develop an all-optical approach to manipulate the charge states of excitons in monolayer molybdenum disulfide (MoS2). Through steering the laser beam, we demonstrate reconfigurable optical encoding of the excitonic charge states (between neutral and negative states) on a single MoS2 flake. Our technique can be extended to other TMDs materials, which will guide the design of all-optical and reconfigurable TMD-based optoelectronic and nanophotonic devices.

Optical Visualization of Photoexcitation Diffusion in All-Inorganic Perovskite at High Temperature.

All-inorganic halide perovskites are promising candidates for optoelectronic and photovoltaic devices because of their good thermal stability and remarkable optoelectronic properties. Among those properties, carrier transport properties are critical as they inherently dominate the device performance. The transport properties of perovskites have been widely studied at room and lower temperatures, but their high-temperature (i.e., tens of degrees above room temperature) characteristics are not fully understood. Here, the photoexcitation diffusion is optically visualized by transient photoluminescence microscopy (TPLM), through which the temperature-dependent transport characteristics from room temperature to 80 °C are studied in all-inorganic CsPbBr3 single-crystalline microplates. We reveal the decreasing trend of diffusion coefficient and the almost unchanged trend of diffusion length when heating the sample to high temperature. The phonon scattering in combination with the variation of effective mass is proposed for the explanation of the temperature-dependent diffusion behavior.

Reconfigurable Metasurface for Image Processing.

Optical Fourier transform-based processing is an attractive technique due to the fast processing times and large-data rates. Furthermore, it has recently been demonstrated that certain Fourier-based processors can be realized in compact form factors using flat optics. The flat optics, however, have been demonstrated as static filters where the operator is fixed, limiting the applicability of the approach. Here, we demonstrate a reconfigurable metasurface that can be dynamically tuned to provide a range of processing modalities including bright-field imaging, low-pass and high-pass filtering, and second-order differentiation. The dynamically tunable metasurface can be directly combined with standard coherent imaging systems and operates with a numerical aperture up to 0.25 and over a 60 nm bandwidth. The ability to dynamically control light in the wave vector domain, while doing so in a compact form factor, may open new doors to applications in microscopy, machine vision, and sensing.

Near-field nonlinear imaging of an anapole mode beyond diffraction limit.

Nonlinear nanophotonics, as an emerging field in nanophotonics, eagerly calls for experimental techniques for probing and analyzing near-field nonlinear optical signals with subwavelength resolution. Here, we report an aperture-type scanning near-field optical microscopic method for probing near-field nonlinear optical processes. As a demonstration, near-field third-harmonic generation from an anapole dark-mode state generated by a silicon nanodisk is probed and imaged. The measured results agree well with the simulations, with a spatial resolution down to $0.14{\lambda _0}$ and a sensitivity of 0.1 nW. This method provides a powerful tool for characterizing nonlinear light-matter interactions at the nanoscale, which can help, for example, to unveil crystal properties involving subwavelength defects or dislocations.

Active Surface with Dynamic Microstructures and Hierarchical Gradient Enabled by in situ Pneumatic Control.

An active surface with an on-demand tunable topography holds great potential for various applications, such as reconfigurable metasurfaces, adaptive microlenses, soft robots and four-dimensional (4D) printing. Despite extensive progress, to achieve refined control of microscale surface structures with large-amplitude deformation remains a challenge. Moreover, driven by the demand of constructing a large area of microstructures with increased complexity-for instance, biomimetic functional textures bearing a three-dimensional (3D) gradient-novel strategies are highly desired. Here, we develop an active surface with a dynamic topography and three-tier height gradient via a strain-tunable mismatching-bonding process. Pneumatic actuation allows for rapid, reversible and uniform regulation of surface microstructures at the centimeter scale. The in-situ modulation facilitates large-amplitude deformation with a maximum tuning range of 185 µm. Moreover, the structural gradient can be modulated by programming the strain value of the bonding process. With our strategy, another two types of surfaces with a four-tier gradient and without gradient were also prepared. By providing active modulation and design flexibility of complicated microstructures, the proposed strategy would unlock more opportunities for a wealth of novel utilizations.

Ultra-smooth micro-optical components of various geometries.

A dry-etching-assisted femtosecond laser lithography technology is proposed to in-site fabricate micro-optical components with an ultra-smooth three-dimensional continuous profile on a non-planar substrate. Owing to the nanometric resolution of femtosecond laser multi-photon polymerization and dry etching, smooth micro-optical components can be realized on hard materials with surface roughness of approximately 1.5 nm. With flexible and arbitrary designability of femtosecond laser lithography, various high-quality micro-optical components are realized on sapphire. These results indicate that dry-etching-assisted femtosecond laser lithography has promising potential for versatile fabrication of arbitrary ultra-smooth micro/nanostructures on hard materials.

Near-field probing the magnetic field vector of visible light with a silicon nanoparticle probe and nanopolarimetry.

Magnetic light-matter interaction plays a crucial role in nanophysics, such as in photonic topological insulators and metamaterials. Recent advances in all-dielectric nanophotonics especially demand vectorial mapping of magnetic light at visible wavelengths. Here, we report that a novel functional nanoprobe decorated with a silicon nanoparticle predominantly senses both the vertical and lateral magnetic field, that is, the magnetic field vector, complementary to a metal nanoparticle probe detecting the local electric field vector. As a proof-of-principle experiment, we demonstrate the mapping of magnetic field vectors in a transverse electric (TE) evanescent standing wave by this probe in a scanning near-field optical microscope (SNOM) with nanopolarimetry. It is for the first time that the full magnetic field vector of visible light, whose frequency exceeds 550 THz, can be directly detected with deep subwavelength resolution. Such functional probe and nanopolarimetry may pave the way toward complete vectorial near-field characterization over the whole visible band for nano-optics and subwavelength optics.

Probing vectorial near field of light: imaging theory and design principles of nanoprobes.

Near-field microscopy is widely used for characterizing electromagnetic fields at nanoscale, where nanoprobes afford the opportunity to extract subwavelength optical quantities, including the amplitude, phase, polarization, chirality, etc. However, owing to the complexity of various nanoprobes, a general and intuitive theory is highly desired to assess the vectorial responses of nanoprobes and interpret the mechanism of the probe-field interaction. Here, we develop a general imaging theory based on the reciprocity of electromagnetism and multipole expansion analysis. The proposed theory closely resembles the multipolar Hamiltonian for light-matter interaction energy, revealing the coupling mechanism of the probe-field interaction. Based on this theory, we introduce a new paradigm for the design of functional nanoprobes by analyzing the reciprocal dipole moments, and establish effective design principles for the imaging of vectorial near fields. As application examples of the proposed theory, we numerically analyze the responses of two typical probes, a split-ring probe and a nanoparticle probe, which can quantitatively reproduce and well explain the experimental results of previously reported measurements of the optical magnetism and the transverse spin angular momentum. Our work provides a powerful tool for the design and analysis of new functional probes that may enable the probing of various physical quantities of the vectorial near field.

General Strategy toward Dual-Scale-Controlled Metallic Micro-Nano Hybrid Structures with Ultralow Reflectance.

Functional metal surfaces with minimum optical reflection over a broadband spectrum have essential importance for optical and optoelectronic devices. However, the intrinsically large optical impedance mismatch between metals and the free space causes a huge obstacle in achieving such a purpose. We propose and experimentally demonstrate a general pulse injection controlled ultrafast laser direct writing strategy for fabricating highly effective antireflection structures on metal surfaces. The presented strategy can implement separate and flexible modifications on both microscale frame structures and nanoscale particles, a benefit from which is that optimized geometrical light trapping and enhanced effective medium effect reducing the surface reflection can be simultaneously achieved within one hybrid structure. Thus, comprehensively improved antireflection performances can be realized. Hybrid structures with substantial nanoparticles hierarchically attached on regularly arrayed microcones are generally constructed on different metal surfaces, achieving highly efficient light absorption over ultraviolet to near-infrared broadband spectrum regions. Reflectance minimums of 1.4%, 0.29%, and 2.5% are reached on Cu, Ti, and W surfaces, respectively. The presented strategy is simple in process, adaptable for different kinds of metals, reproduceable in dual-scale structural features, and feasible for large-area production. All these advantages make the strategy as well as the prepared antireflection structures excellent candidates for practical applications.

Ultra-thin and high-efficiency graphene metasurface for tunable terahertz wave manipulation.

We propose a type of ultra-thin metasurfaces composed of rectangular graphene patches supporting orthogonal plasmonic resonances, which can work in transmission or reflection modes for dynamic terahertz wavefront manipulation with high polarization conversion ratio. By controlling the response of each patch via electrical biasing, the phase of the output wave can be tuned in a wide range over 180° while keeping its amplitude high and relatively stable. We demonstrate several functional devices based on such metasurfaces: a linear polarization converter with nearly 100% polarization conversion ratio, a switchable anomalous wave deflection device, and a dual-polarity focusing mirror with the focal spot tunable in both the transversal and longitudinal directions.

Versatile and tunable surface plasmon polariton excitation over a broad bandwidth with a simple metaline by external polarization modulation.

Surface plasmon polariton (SPP) sources and launchers are highly demanded in various applications of nanophotonics. Here, we propose a general approach that can realize complete control of the complex extinction ratio (including amplitude and phase) of any two linearly independent SPP modes excited by any elementary SPP excitation architecture just by manipulating the incident polarization state. In an optical system, it suffices to simply tune the orientation angles of a linear polarizer and a quarter wave plate, which may greatly simplify the design and application of SPP launchers and diversify their functionalities. As an example to show the broad application prospect of this method, we design and realize a metaline consisting of Δ-shaped plasmonic nanoantennas, which can effectively realize dual functionalities, i.e., the tunable directional SPP excitation at an arbitrarily chosen wavelength and the complete unidirectional SPP excitation over a broad bandwidth. This general approach can also be extended to the control of the complex extinction ratio of any two linearly independent excited modes in many other linear optical systems, such as two modes in a waveguide or two diffraction orders in a grating, over a broad bandwidth.

Large-scale cauliflower-shaped hierarchical copper nanostructures for efficient photothermal conversion.

Efficient solar energy harvesting and photothermal conversion have essential importance for many practical applications. Here, we present a laser-induced cauliflower-shaped hierarchical surface nanostructure on a copper surface, which exhibits extremely high omnidirectional absorption efficiency over a broad electromagnetic spectral range from the UV to the near-infrared region. The measured average hemispherical absorptance is as high as 98% within the wavelength range of 200-800 nm, and the angle dependent specular reflectance stays below 0.1% within the 0-60° incident angle. Such a structured copper surface can exhibit an apparent heating up effect under the sunlight illumination. In the experiment of evaporating water, the structured surface yields an overall photothermal conversion efficiency over 60% under an illuminating solar power density of ∼1 kW m(-2). The presented technology provides a cost-effective, reliable, and simple way for realizing broadband omnidirectional light absorptive metal surfaces for efficient solar energy harvesting and utilization, which is highly demanded in various light harvesting, anti-reflection, and photothermal conversion applications. Since the structure is directly formed by femtosecond laser writing, it is quite suitable for mass production and can be easily extended to a large surface area.

Fast and Simultaneous Determination of the Number and Mass Concentrations of Gold Nanorod Colloid Using an Improved Optical Extinction-Scattering Spectroscopic Method.

Accurate determination of the concentrations, including the mass concentration (MC) and number concentration (NC), of metal nanoparticle (NP) colloid is highly demanded in the synthesis, metrology, and application of NPs. The commonly used inductively coupled plasma mass spectrometry (ICP-MS) can only measure the MC of NPs, which is destructive to the NPs and requires advanced operation skills. Here, we present a simple approach based on an improved optical extinction-scattering spectroscopic (OESS) method to fast determining the MC and NC of metal nanorod colloids simultaneously. Unlike most existing spectroscopic methods that can only deal with low-concentration NP colloids, the improved OESS method can accurately solve the inverse scattering problem of NP colloids with higher concentrations, so that a two-dimensional joint probability density function of both the width and aspect ratio of nanorods can be retrieved, which makes the basis for the accurate determination of the MC and NC of the colloids in a large range of concentration. The reliability and accuracy of the method are validated by measuring several typical nanorod colloids with different concentrations and comparing the results with those obtained by the standard ICP-MS method. It is shown that the improved OESS method can cover a broad MC measurement range of at least 10-50 µg/mL and a NC measurement range of 10(9)-10(11)/mL. The uncertainty and sources of error in the measurement are also analyzed. Since the improved OESS method is fast, cost-effective, non-destructive, and easy to implement, it provides a simple way to determine the concentrations of metal NPs and has the potential to be extended to other metal NPs.

A simple method for generating unidirectional surface plasmon polariton beams with arbitrary profiles.

The efficient steering of surface plasmon polariton (SPP) fields is a vital issue in various plasmonic applications, such as plasmonic circuitry. We present a straightforward and efficient method for generating unidirectionally propagating SPP beams with arbitrary amplitude and phase profiles by manipulating Δ-shaped nanoantennas. As an example, a second-order Hermite-Gauss SPP beam is generated with this method. The near-field distribution of the generated SPP beam is experimentally characterized to validate the effectiveness of the method.

Broadband Hybrid Holographic Multiplexing with Geometric Metasurfaces.

An effective way for broadband holographic multiplexing based on geometric metasurfaces is demonstrated by the integration of several recording channels into a single device. Each image can be individually addressed with a unique set of parameters, such as circular polarization, position, and angle. Such a technique paves the way for a wide range of applications related to optical patterning, encryption, and information processing.

Dual-wavelength extinction method for fast sizing of metal nanosphere ensembles.

We propose a simple dual-wavelength extinction (DWE) method to measure the average size of spherical metal nanoparticle (NP) ensembles. Unlike the spectroscopic methods that need to measure the full spectra of scattering and/or extinction to retrieve the NP size, the DWE method can estimate the NP size by measuring the light extinction at only two properly selected wavelengths and thus is useful for fast sizing of metal NP ensembles. The influences of the NP shape deviation and ensemble dispersancy on the measurement accuracy are analyzed and discussed in detail. An empirical correction procedure is established to compensate these influences to further improve accuracy. The feasibility and reliability of the DWE method are corroborated by experimentally measuring several typical gold spherical NP ensembles and comparing the results with those obtained by three other standard methods. The experimental results indicate satisfactory accuracy of the DWE method for measuring gold NPs from 30 to 100 nm by using two measurement wavelengths of 532 and 573 nm. The studies show that the DWE method is efficient, reliable, and easy to implement. It may find wide applications in the metrology of NPs.

Broadband High-Performance Infrared Antireflection Nanowires Facilely Grown on Ultrafast Laser Structured Cu Surface.

Infrared antireflection is an essential issue in many fields such as thermal imaging, sensors, thermoelectrics, and stealth. However, a limited antireflection capability, narrow effective band, and complexity as well as high cost in implementation represent the main unconquered problems, especially on metal surfaces. By introducing precursor micro/nano structures via ultrafast laser beforehand, we present a novel approach for facile and uniform growth of high-quality oxide semiconductor nanowires on a Cu surface via thermal oxidation. Through the enhanced optical phonon dissipation of the nanowires, assisted by light trapping in the micro structures, ultralow total reflectance of 0.6% is achieved at the infrared wavelength around 17 µm and keeps steadily below 3% over a broad band of 14-18 µm. The precursor structures and the nanowires can be flexibly tuned by controlling the laser processing procedure to achieve desired antireflection performance. The presented approach possesses the advantages of material simplicity, structure reconfigurability, and cost-effectiveness for mass production. It opens a new path to realize unique functions by integrating semiconductor nanowires onto metal surface structures.

M-shaped grating by nanoimprinting: a replicable, large-area, highly active plasmonic surface-enhanced Raman scattering substrate with nanogaps.

Plasmonic nanostructures separated by nanogaps enable strong electromagnetic-field confinement on the nanoscale for enhancing light-matter interactions, which are in great demand in many applications such as surface-enhanced Raman scattering (SERS). A simple M-shaped nanograting with narrow V-shaped grooves is proposed. Both theoretical and experimental studies reveal that the electromagnetic field on the surface of the M grating can be pronouncedly enhanced over that of a grating without such grooves, due to field localization in the nanogaps formed by the narrow V grooves. A technique based on room-temperature nanoimprinting lithography and anisotropic reactive-ion etching is developed to fabricate this device, which is cost-effective, reliable, and suitable for fabricating large-area nanostructures. As a demonstration of the potential application of this device, the M grating is used as a SERS substrate for probing Rhodamine 6G molecules. Experimentally, an average SERS enhancement factor as high as 5×108 has been achieved, which verifies the greatly enhanced light-matter interaction on the surface of the M grating over that of traditional SERS surfaces.