Near-field Properties Research Articles

Verification of a metamaterial with gradient particles and its near-field radiative heat transfer property

Verification of a metamaterial with gradient particles and its near-field radiative heat transfer property

Polarization-independent tetramer metastructure with multi-Fano resonances governed by quasi-bound states in the continuum

We propose what we believe to be a novel metastructure consisting of silicon nanoblock tetramer clusters and investigated theoretically and experimentally how to enhance surface sensing capabilities with polarization-independent properties through bound states in the continuum (BICs). By introducing square defects, three quasi-BIC modes are excited at the wavelengths of 1013.29 nm, 1109.57 nm, and 1310.73 nm with a modulation depth up to 100% and a Q-factor of 16618, while achieving a sensitivity of 256 nm/RIU and a figure of merit of 2519.7 RIU−1. Utilizing the finite-difference method in the time domain (FDTD), we have analyzed the electromagnetic near-field distributions, polarization properties, and robustness corresponding to resonance dips at different wavelengths. Our results reveal that the distinct electromagnetic near-field distributions excited by the quasi-BIC modes are characterized by the strong field confinement within the silica nanoblock tetramer clusters. The modes are primarily governed by magnetic quadrupole (MQ) resonance and toroidal dipole (TD) moment. Additionally, the polarization-independent properties of the metastructure are demonstrated to ensure that they can effectively respond to the incident light regardless of its polarization state, while the robustness is investigated to show the stability and reliability by shifting square defects. Moreover, the transmission spectra of the metastructure is experimentally verified by immersing the sample into CaCl2 solutions in different concentrations. This work plays a pivotal role in creating further novel and high-performance optical metastructures while demonstrating the potential applications of quasi-BIC modes in precision sensing in the future.

Distribution of Single-Particle Resonances Determines the Plasmonic Response of Disordered Nanoparticle Ensembles.

Understanding how colloidal soft materials interact with light is crucial to the rational design of optical metamaterials. Electromagnetic simulations are computationally expensive and have primarily been limited to model systems described by a small number of particles-dimers, small clusters, and small periodic unit cells of superlattices. In this work we study the optical properties of bulk, disordered materials comprising a large number of plasmonic colloidal nanoparticles using Brownian dynamics simulations and the mutual polarization method. We investigate the far-field and near-field optical properties of both colloidal fluids and gels, which require thousands of nanoparticles to describe statistically. We show that these disordered materials exhibit a distribution of particle-level plasmonic resonance frequencies that determines their ensemble optical response. Nanoparticles with similar resonant frequencies form anisotropic and oriented clusters embedded within the otherwise isotropic and disordered microstructures. These collectively resonating morphologies can be tuned with the frequency and polarization of incident light. Knowledge of particle resonant distributions may help to interpret and compare the optical responses of different colloidal structures, correlate and predict optical properties, and rationally design soft materials for applications harnessing light.

Substrate-induced hybridization of plasmon modes in the composite nanostructure of nanodisk array/thin film for spectrum modulation

Abstract Hybridization coupling among plasmon modes is an effective approach to manipulate near-field properties thus optical spectral shapes of plasmonic nanostructures. Generally, mode hybridization coupling is achieved by modifying the topography and dimensions of nanostructures themselves, with few concerns about substrate-induced manipulation. Herein, we propose a composite nanostructure consisting of a gold (Au) nanodisk array and a thin Au film supported by a dielectric substrate. In this configuration, both the refractive index of the dielectric substrate and thin gold film’s thickness mediate the interaction of plasmon modes supported by upper and lower interfaces of the composite nanostructure, resulting in two hybridized plasmon modes. We systematically investigate the relationship between optical fields at the top surface of plasmon modes before and after the hybridization coupling. Specifically, the near-field amplitude at the top surface of the unhybridized modes is stronger than that of individual hybridized mode, and lower than the near-field summation of these two hybridized modes. This work not only provides a straightforward strategy for generating two plasmon modes in a nanostructure but also elucidates the variation of the optical field during the hybridization process, which is of crucial significance for applications, such as upconversion enhancement and multi-resonance sensing.

Surface-Enhanced Raman Spectroscopy of Ammonium Nitrate Using Al Structures, Fabricated by Laser Processing of AlN Ceramic.

This work presents results on laser-induced surface structuring of AlN ceramic and its application in Surface-Enhanced Raman Spectroscopy (SERS). The laser processing is performed by nanosecond pulses in air and vacuum. Depending on the processing conditions, different surface morphology can be obtained. The ablation process is realized by ceramic decomposition as the formation of an aluminium layer is detected. The efficiency of the fabricated structures as active substrates in SERS is estimated by the ability of the detection of ammonium nitrate (NH4NO3). It is conducted for Raman spectrometer systems that operate at wavelengths of 514 and 785 nm where the most common commercial systems work. The obtained structures contribute to enhancement of the Raman signal at both wavelengths, as the efficiency is higher for excitation at 514 nm. The limit of detection (LOD) of ammonium nitrate is estimated to be below the maximum allowed value in drinking water. The analysis of the obtained results was based on the calculations of the near field enhancement at different conditions based on Finite Difference Time Domain simulation and the extinction spectra calculations based on Generalized Mie scattering theory. The structures considered in these simulations were taken from the SEM images of the real samples. The oxidation issue of the ablated surface was studied by X-ray photoelectron spectroscopy. The presented results indicated that laser structuring of AlN ceramics is a way for fabrication of Al structures with specific near-field properties that can be used for the detection of substances with high social impact.

Tuning the Geometry and Optical Chirality of Pentatwinned Au Nanoparticles with 5-Fold Rotational Symmetry.

Chirality transfer from chiral molecules to chiral nanomaterials represents an important topic for exploring the origin of chirality in many natural and artificial systems. Moreover, developing a promising class of chiral nanomaterials holds great significance for various applications, including sensing, photonics, catalysis, and biomedicine. Here we demonstrate the geometric control and tunable optical chirality of chiral pentatwinned Au nanoparticles with 5-fold rotational symmetry using the seed-mediated chiral growth method. A distinctive growth pathway and optical chirality are observed using pentatwinned decahedra as seeds, in comparison with the single-crystal Au seeds. By employing different peptides as chiral inducers, pentatwinned Au nanoparticles with two distinct geometric chirality (pentagonal nanostars and pentagonal prisms) are obtained. The intriguing formation and evolution of geometric chirality with the twinned structure are analyzed from a crystallographic perspective upon maneuvering the interplay of chiral molecules, surfactants, and reducing agents. Moreover, the interesting effects of the molecular structure of peptides on tuning the geometric chirality of pentatwinned Au nanoparticles are also explored. Finally, we theoretically and experimentally investigate the far-field and near-field optical properties of chiral pentatwinned Au nanoparticles through numerical simulations and single-particle chiroptical measurements. The ability to tune the geometric chirality in a controlled manner represents an important step toward the development of chiral nanomaterials with increasing architectural complexity for chiroptical applications.

A recursive cell multipole method for atomistic electrodynamics models.

For large plasmonic nanoparticles, retardation effects become important once their length becomes comparable to the wavelength of light. However, most models do not incorporate retardation effects due to the high computational cost of solving for the optical properties of large atomistic electrodynamics systems. In this work, we derive and implement a recursive fast multipole method (FMM) in Cartesian coordinates that includes retardation effects. In this method, higher-order electrodynamic interaction tensors used for the FMM are calculated recursively, thus greatly reducing the implementation complexity of the model. This method allows for solving of the optical properties of large atomistic nanoparticles with controlled accuracy; in practice, taking the expansion to the fifth order provides a good balance of accuracy and computational time. Finally, we study the effects retardation has on the near- and far-field properties of large plasmonic nanoparticles with over a million atoms using this method. We specifically focus on nanorods and their dimers, which are known to generate highly confined fields in their junctions. In the future, this method can be applied to simulations in which accurate near-field properties are required, such as surface-enhanced Raman scattering.

Footprints of scanning probe microscopy on halide perovskites.

Scanning probe microscopy (SPM) and advanced atomic force microscopy (AFM++) have become pivotal for nanoscale elucidation of the structural, optoelectronic and photovoltaic properties of halide perovskite single crystals and polycrystalline films, both under ex situ and in situ conditions. These techniques reveal detailed information about film topography, compositional mapping, charge distribution, near-field electrical behaviors, cation-lattice interactions, ion dynamics, piezoelectric characteristics, mechanical durability, thermal conductivity, and magnetic properties of doped perovskite lattices. This article outlines the advancements in SPM techniques that deepen our understanding of the optoelectronic and photovoltaic performances of halide perovskites.

Distortions in focusing laser pulses due to spatio-temporal couplings: an analytic description

Abstract In ultra-short laser pulses, small changes in dispersion properties before the final focusing mirror can lead to severe pulse distortions around the focus and therefore to very different pulse properties at the point of laser–matter interaction, yielding unexpected interaction results. The mapping between far- and near-field laser properties intricately depends on the spatial and angular dispersion properties as well as the focal geometry. For a focused Gaussian laser pulse under the influence of angular, spatial and group-delay dispersion, we derive analytical expressions for its pulse-front tilt, duration and width from a fully analytic expression for its electric field in the time–space domain obtained with scalar diffraction theory. This expression is not only valid in and near the focus but also along the entire propagation distance from the focusing mirror to the focus. Expressions relating angular, spatial and group-delay dispersion before focusing at an off-axis parabola, where they are well measurable, to the respective values in the pulse’s focus are obtained by a ray tracing approach. Together, these formulas are used to show in example setups that the pulse-front tilts of lasers with small initial dispersion can become several tens of degrees larger in the vicinity of the focus while being small directly in the focus. The formulas derived here provide the analytical foundation for observations previously made in numerical experiments. By numerically simulating Gaussian pulse propagation and measuring properties of the pulse at distances several Rayleigh lengths off the focus, we verify the analytic expressions.

Generation of Vortex Beams via All-Dielectric Spin-Multiplexed Coding Metamaterials

The vector vortex beams are generated by the single-phase modulation of metasurfaces, which severely limits the freedom of design. We use the combination of the propagation phase and the geometric phase to construct a transmissive all-dielectric encoded metasurface. Under two orthogonal circularly polarized incidence conditions, vortex beams with different topological charge can be generated. We utilize the hybrid-order Poincaré sphere to characterize various polarization states of Poincaré vortex beams. Based on the near-field and far-field intensity distribution and phase distribution properties of the vortex beam, the design accuracy of the Poincaré vortex beam is confirmed. In order to improve the degree of freedom of control of vortex beams, we introduce the Fourier convolution principle in digital signal processing. The convolution operation of the encoding array and the phase gradient sequence is performed to construct a new encoding metasurface sequence, and the scattering angle of the vortex beam can be adjusted. Using the principle of coded convolution, functions with arbitrary deflection and beam splitting of vortex beams can be realized.

Multi-wavelength unidirectional forward scattering properties of the arrow-shaped galliumphosphide nanoantenna.

An arrow-shaped gallium phosphide nanoantenna exhibits both near-field electric field enhancement and far-field unidirectional scattering, and the interference conditions involve electric and magnetic quadrupoles as well as toroidal dipoles. By using long-wavelength approximation and exact multipole decomposition, the interference conditions required for far-field unidirectional transverse light scattering and backward near-zero scattering at multiple wavelengths are determined. The near-field properties are excellent, as exemplified by large Purcell factors of 4.5×109 for electric dipole source excitation, 464.68 for magnetic dipole source excitation, and 700V/m for the field enhancement factor. The degree of enhancement of unidirectional scattering is affected by structural parameters such as the angle and thickness of the nanoantenna. The arrow-shaped nanoantenna is an efficient platform to enhance the electric field and achieve high directionality of light scattering. Moreover, the nanostructure enables flexible manipulation of light waves and materials, giving rise to superior near-field and far-field performances, which are of great importance pertaining to the practicability and application potential of optical antennas in applications such as spectroscopy, sensing, displays, and optoelectronic devices.

The Effect of Nanoparticle Composition on the Surface-Enhanced Raman Scattering Performance of Plasmonic DNA Origami Nanoantennas.

A versatile generation of plasmonic nanoparticle dimers for surface-enhanced Raman scattering (SERS) is presented by combining a DNA origami nanofork and spherical and nonspherical Au or Ag nanoparticles. Combining different nanoparticle species with a DNA origami nanofork to form DNA origami nanoantennas (DONAs), the plasmonic nanoparticle dimers can be optimized for a specific excitation wavelength in SERS. The preparation of such nanoparticle dimers is robust enough to enable the characterization of SERS intensities and SERS enhancement factors of dye-modified DONAs on a single dimer level by measuring in total several thousands of dimers from five different dimer designs, each functionalized with three different Raman reporter molecules and measured at four different excitation wavelengths. Based on these data, SERS enhancement factor (EF) distributions have been determined for each dimer design and excitation wavelengths. The structures and measurement conditions with the highest EFs are suitable for single-molecule SERS (SM-SERS), which is realized by placing single dye molecules into hot spots. We demonstrate that the probability of placing single molecules in a strongly enhancing hot spot for SM-SERS can be increased by using anisotropic nanoparticles with several sharp edges, such as nanoflowers. Combining a Ag nanoparticle with a Au particle in one dimer structure allows for a broadband excitation covering almost the whole visible range. The most versatile plasmonic dimer structure for SERS combines a spherical Ag nanoparticle with a Au nanoflower. Employing the discontinuous Galerkin time domain method, we numerically investigate the bare, symmetric dimers with respect to spectral and near-field properties, showing that, indeed, the nanoflowers induce multiple hot spots located at the edges which surpass the intensity of the spherical dimers, indicating the possibility for SM-SERS. The presented DONA structures and SERS data provide a robust basis for applying such designs as versatile SERS tags and as substrates for SM-SERS measurements.

Cryogenic Hydrogen Jet and Flame for Clean Energy Applications: Progress and Challenges

Industries across the world are making the transition to net-zero carbon emissions, as government policies and strategies are proposed to mitigate the impact of climate change on the planet. As a result, the use of hydrogen as an energy source is becoming an increasingly popular field of research, particularly in the aviation sector, where an alternative, green, renewable fuel to the traditional hydrocarbon fuels such as kerosene is essential. Hydrogen can be stored in multiple ways, including compressed gaseous hydrogen, cryo-compressed hydrogen and cryogenic liquid hydrogen. The infrastructure and storage of hydrogen will play a pivotal role in the realisation of large-scale conversion from traditional fuels, with safety being a key consideration. This paper provides a review on previous work undertaken to study the characterisation of both unignited and ignited hydrogen jets, which are fundamental phenomena for the utilisation of hydrogen. This includes work that focuses on the near-field flow structure, dispersion in the far-field, ignition and flame characteristics with multi-physics. The safety considerations are also included. The theoretical models and computational fluid dynamics (CFD) multiphase and reactive flow approaches are discussed. Then, an overview of previous experimental work is provided, before focusing the review on the existing computational results, with comparison to experiments. Upon completion of this review, it is highlighted that the complex near-field physics and flow phenomena are areas lacking in research. The near-field flow properties and characteristics are of significant importance with respect to the ignition and combustion of hydrogen.

Optical Chirality of Gold Chiral Helicoid Nanoparticles in the Strong Coupling Region

The far- and near-field chirality properties are usually characterized by circular dichroism (CD) and optical chirality (OC), respectively. As a light–matter interaction for the hybrid states consisting of plasmons and excitons, the strong coupling interactions can affect the original chiral electromagnetic modes. However, there are few works on this influence process, which prevents an in-depth understanding of chirality. Here, we theoretically investigate both the far-field and near-field characteristics of the chiral plasmonic gold helicoid nanoparticle (GHNP) to explore the chirality mechanism further. We found that the electromagnetic field distribution of GHNP consists of one dark mode and two bright modes. The dark mode is observed more clearly in CD than in extinction spectra. Two bright modes can strongly couple with excitons respectively, which is confirmed by the anticrossing behavior and mode splitting exhibited in the extinction and CD spectra. We also analyzed the near-field OC distribution of the GHNP hybrid system and obtained the chiral responses as well as the spectral correspondence between OC and CD. Furthermore, although the strong coupling interaction changes the energy levels, resulting in mode splitting, the chiral hotspot distributions of both the upper polariton branch and lower polariton branch are consistent with the original bright mode in OC maps. Our findings provide guidance for the design of structures with strong chiral responses and enhance the comprehension of chiral strong coupling systems.

Modular mixing in plasmonic metal oxide nanocrystal gels with thermoreversible links.

Gelation offers a powerful strategy to assemble plasmonic nanocrystal networks incorporating both the distinctive optical properties of constituent building blocks and customizable collective properties. Beyond what a single-component assembly can offer, the characteristics of nanocrystal networks can be tuned in a broader range when two or more components are intimately combined. Here, we demonstrate mixed nanocrystal gel networks using thermoresponsive metal-terpyridine links that enable rapid gel assembly and disassembly with thermal cycling. Plasmonic indium oxide nanocrystals with different sizes, doping concentrations, and shapes are reliably intermixed in linked gel assemblies, exhibiting collective infrared absorption that reflects the contributions of each component while also deviating systematically from a linear combination of the spectra for single-component gels. We extend a many-bodied, mutual polarization method to simulate the optical response of mixed nanocrystal gels, reproducing the experimental trends with no free parameters and revealing that spectral deviations originate from cross-coupling between nanocrystals with distinct plasmonic properties. Our thermoreversible linking strategy directs the assembly of mixed nanocrystal gels with continuously tunable far- and near-field optical properties that are distinct from those of the building blocks or mixed close-packed structures.

Some New Results on Near Fields

In this paper, we considered investigating some properties of near fields and new results are obtained. In particular, we investigated some conditions under which some near rings become near fields.

Optical Properties of Ag Nanoparticle Arrays: Near-Field Enhancement and Photo-Thermal Temperature Distribution.

The near-field and photo-thermal properties of nanostructures have always been the focus of attention due to their wide applications in nanomaterials. In this work, we numerically investigate the near-field and photo-thermal temperature distribution in a nanoparticle array when the scattering light field among particles is considered. 'Hot spots', which represent strong electric field enhancement, were analyzed at the difference of the particle size, particle spacing and the polarization direction of the incident light. Interestingly, it is found that the position of the 'hot spots' does not rotate with the polarization direction of the incident light and always remains in the particle gaps along the line between particle centers. Moreover, the near-field is independent of the polarization in some special areas, and the factor of near-field enhancement keeps constant in these spots when the illumination polarization varies. As for photo-induced heating, our results show that both the temperature of the structure center and maximum temperature increase linearly with the particle number of the array while decreasing with the increase in particle spacing. This work provides some theoretical considerations for the near-field manipulation and photo-thermal applications of nanoarrays.

Hybrid Lattice-Boltzmann-Potential Flow Simulations of Turbulent Flow around Submerged Structures

We report on the development and validation of a 3D hybrid Lattice Boltzmann Model (LBM), with Large Eddy Simulation (LES), to simulate the interactions of incompressible turbulent flows with ocean structures. The LBM is based on a perturbation method, in which the velocity and pressure are expressed as the sum of an inviscid flow and a viscous perturbation. The far- to near-field flow is assumed to be inviscid and represented by potential flow theory, which can be efficiently modeled with a Boundary Element Method (BEM). The near-field perturbation flow around structures is modeled by the Navier–Stokes (NS) equations, based on a Lattice Boltzmann Method (LBM) with a Large Eddy Simulation (LES) of the turbulence. In the paper, we present the hybrid model formulation, in which a modified LBM collision operator is introduced to simulate the viscous perturbation flow, resulting in a novel perturbation LBM (pLBM) approach. The pLBM is then extended for the simulation of turbulence using the LES and a wall model to represent the viscous/turbulent sub-layer near solid boundaries. The hybrid model is first validated by simulating turbulent flows over a flat plate, for moderate to large Reynolds number values, Re ∈[3.7×104;1.2×106]; the plate friction coefficient and near-field turbulence properties computed with the model are found to agree well with both experiments and direct NS simulations. We then simulate the flow past a NACA-0012 foil using a regular LBM-LES and the new hybrid pLBM-LES models with the wall model, for Re = 1.44×106. A good agreement is found for the computed lift and drag forces, and pressure distribution on the foil, with experiments and results of other numerical methods. Results obtained with the pLBM model are either nearly identical or slightly improved, relative to those of the standard LBM, but are obtained in a significantly smaller computational domain and hence at a much reduced computational cost, thus demonstrating the benefits of the new hybrid approach.

Control infrastructure monitoring system at the NSRL facility cluster

The National Synchrotron Radiation Laboratory (NSRL) facility cluster is a collection of user facilities developed by NSRL, including the Hefei Light Source-II (HLS-II), Tunable Infrared Laser for Fundamental of Energy Chemistry (FELiChEM), and THz near-field high-flux material physical property test system (NFTHZ). User facilities generally have high operational availability requirements. The NSRL facility cluster relies on the control infrastructure to provide computing, network, and storage resources, as well as various services that must be available 24 hours a day, 7 days a week. The monitoring system is responsible for tracking the operational status of the control infrastructure, gathering information on faults, performance degradation and cybersecurity issues, and distributing alarm messages in time. It facilitates the operator troubleshooting problems efficiently to improve the availability of the user facilities. The monitoring system is developed by integrating several free and open source software tools. Zabbix is selected as the monitoring tool and collects metrics data from the control infrastructure. Three upper-layer applications are developed for data visualization. The dashboard shows the operational status of the network and various devices. The alarm system collects and distributes alarm messages via web-based GUI and WeChat. The reporting system periodically generates metrics and alarm reports. The monitoring system has been deployed since March 2022. The results indicate that the monitoring system can effectively identify hidden hazards in the control infrastructure.

Plasmon resonance of gold and silver nanoparticle arrays in the Kretschmann (attenuated total reflectance) vs. direct incidence configuration

While the behaviour of plasmonic solid thin films in the Kretschmann (also known as Attenuated Total Reflection, ATR) configuration is well-understood, the use of discrete nanoparticle arrays in this optical configuration is not thoroughly explored. It is important to do so, since close packed plasmonic nanoparticle arrays exhibit exceptionally strong light-matter interactions by plasmonic coupling. The present work elucidates the optical properties of plasmonic Au and Ag nanoparticle arrays in both the direct normal incidence and Kretschmann configuration by numerical models, that are validated experimentally. First, hexagonal close packed Au and Ag nanoparticle films/arrays are obtained by air–liquid interfacial assembly. The numerical models for the rigorous solution of the Maxwell’s equations are validated using experimental optical spectra of these films before systematically investigating various parameters. The individual far-field/near-field optical properties, as well as the plasmon relaxation mechanism of the nanoparticles, vary strongly as the packing density of the array increases. In the Kretschmann configuration, the evanescent fields arising from p- and s-polarized (or TM and TE polarized) incidence have different directional components. The local evanescent field intensity and direction depends on the polarization, angle of incidence and the wavelength of incidence. These factors in the Kretschmann configuration give rise to interesting far-field as well as near-field optical properties. Overall, it is shown that plasmonic nanoparticle arrays in the Kretschmann configuration facilitate strong broadband absorptance without transmission losses, and strong near-field enhancement. The results reported herein elucidate the optical properties of self-assembled nanoparticle films, pinpointing the ideal conditions under which the normal and the Kretschmann configuration can be exploited in multiple light-driven applications.