The optical response of materials based on gold nanoparticle assemblies depends on many parameters regarding both material morphology and light excitation characteristics. In this paper, the interplay between the optical and thermal responses of such media is particularly investigated under its theoretical aspect. Both conventional and original modeling approaches are presented and applied to concrete cases. We first show how the interaction of light with matrix-embedded gold nanoparticles can result in the generation of thermal excitations through different energy exchange mechanisms. We then describe how thermal processes can affect the optical response of a nanoparticle assembly. Finally, we connect both aspects and point out their involvement in the nonlinear optical response of nanocomposite media. This allows us to tackle two key issues in the field of third-order nonlinear properties of gold nanoparticles: The influence of the generalized thermal lens in the long laser pulse regime and the hot electron contribution to the gold particle intrinsic third-order susceptibility, including its spectral dispersion and intensity-dependence. Additionally, we demonstrate the possible significant influence of the heat carrier ballistic regime and phonon rarefaction in the cooling dynamics of an embedded gold nanoparticle subsequent to ultrafast pulsed laser excitation.
We demonstrate the application of machine learning for rapid and accurate extraction of plasmonic particles cluster geometries from hyperspectral image data via a dual variational autoencoder (dual-VAE). In this approach, the information is shared between the latent spaces of two VAEs acting on the particle shape data and spectral data, respectively, but enforcing a common encoding on the shape-spectra pairs. We show that this approach can establish the relationship between the geometric characteristics of nanoparticles and their far-field photonic responses, demonstrating that we can use hype…
Melanin is a ubiquitous natural pigment that exhibits broadband absorption and high refractive index. Despite its widespread use in structural color production, how the absorbing material, melanin, affects the generated color is unknown. Using a combined molecular dynamics and finite-difference time-domain computational approach, this paper investigates structural color generation in one-component melanin nanoparticle-based supra-assemblies (called supraballs) as well as binary mixtures of melanin and silica (non-absorbing) nanoparticle-based supraballs. Experimentally produced one-component m…
Spatially Uniform and Defect-Tolerant Plasmonic Responses in 3D printed Gold Nanoparticle Assemblies
Paderborn University（帕德博恩大学）；Kumoh National Institute of Technology（龟尾国立科学技术院）；Gumi Electronics & Information Technology Research Institute（龟尾电子信息技术研究院）；Hallym University（韩国基督教大学）
Gold nanoparticles are unique electrocatalysts for oxygen reduction, carbon dioxide reduction, and alcohol oxidation. Electrocatalytic processes are influenced by the interaction with the solvent, yet the direct investigation of the solvation of nanoparticles is scarce. Here we select gold nanoparticles as 10 nm sized solutes of which we can control the charge. We perform mid-infrared and terahertz spectroscopy to compare the behavior of the water in solution with micelles loaded with neutral and positive gold nanoparticles. We find indications that the hydration water around the gold-loaded m…
The Photothermal Heterodyne Imaging method is used to study for the first time the absorption spectra of individual gold nanoparticles with diameters down to 5 nm. Intrinsic size effects wich result in a broadening of the Surface Plasmon resonance are unambiguously observed. Dispersions in the peak energies and homogeneous widths of the single particle resonances are revealed. The experimental results are analysed within the frame of Mie theory.
We introduce TERMS, an open-source Fortran program to simulate near-field and far-field optical properties of clusters of particles. The program solves rigorously the Maxwell equations via the superposition T-matrix method, where incident and scattered fields are decomposed into series of vector spherical waves. TERMS implements several algorithms to solve the coupled system of multiple scattering equations that describes the electromagnetic interaction between neighbouring scatterers. From this formal solution, the program can compute a number of physically-relevant optical properties, such a…
This paper describes an imaging microscopic technique based on heterodyne digital holography where subwavelength-sized gold colloids can be imaged in cell environment. Surface cellular receptors of 3T3 mouse fibroblasts are labeled with 40 nm gold nanoparticles, and the biological specimen is imaged in a total internal reflection configuration with holographic microscopy. Due to a higher scattering efficiency of the gold nanoparticles versus that of cellular structures, accurate localization of a gold marker is obtained within a 3D mapping of the entire sample's scattered field, with a lateral…
The homogenization of vaterite impregnated with gold nanoparticles was accomplished using the extended Maxwell Garnett formalism. The extended formalism takes into account the intrinsic anisotropy of vaterite as well as the size, shape, and orientation of the nanoparticles. Size-dependent permittivity was used for the gold nanoparticles. Numerical studies revealed that the homogenized composite material's permittivity parameters are acutely sensitive to the size, shape, orientation, and volume fraction of the gold nanoparticles.
In this work we use femtosecond laser pulses of 800 nm wavelength to excite and characterize the multiphoton luminescence emission of single gold nanoparticles. For excitation with 100 fs laser pulses we observe a two and three photon emission dominated by radiative electron hole pair recombination, while the emission is caused by radiative plasmon decay for excitation with 500 fs pulses. For single gold nanorods with different aspect ratios, we study the interplay between the particle plasmon and electron hole pairs, which enables us to develop a quantitative model to fully describe the two a…
We report on highly nonlinear luminescence being observed from individual spherical gold nanoparticles immobilized on a glass surface and illuminated by continuous-wave (CW) lasers with relatively low power. The nonlinear luminescence shows optical super-resolution beyond the diffraction limit in three dimensions compared to the scatting of the excitation laser light. The luminescence intensity from most nanoparticles is proportional to the 5th--7th power of the excitation laser power and has wide excitation and emission spectra across the visible wavelength range. Strong nonlinear luminescenc…
We present a new technique that combines off-axis Digital Holography and Dark Field Microscopy to track 100nm gold particles diffusing in water. We show that a single hologram is sufficient to localize several particles in a thick sample with a localization accuracy independent of the particle position. From our measurements we reconstruct the trajectories of the particles and derive their 3D diffusion coefficient. Our results pave the way for quantitative studies of the motion of single nanoparticle in complex media.
Graphene covered metal nanoparticles constitute a novel type of hybrid materials, which provide a unique platform to study plasmonic effects, surface-enhanced Raman scattering (SERS), and metal-graphene interactions at the nanoscale. Such a hybrid material is fabricated by transferring graphene grown by chemical vapor deposition onto closely spaced gold nanoparticles produced on a silica wafer. The morphology and physical properties of nanoparticle-supported graphene is investigated by atomic force microscopy, optical reflectance spectroscopy, scanning tunneling microscopy and spectroscopy (ST…
In this letter, we demonstrate the integration of short metal nanoparticle chains (L \approx 700nm) supporting localized surface plasmons in Silicon On Insulator (SOI) waveguides at telecom wavelengths. Nanoparticles are deposited on the waveguide top and excited through the evanescent field of the TE waveguide modes. Finite difference time domain calculations and waveguide transmission measurements reveal that almost all the TE mode energy can be transferred to nanoparticle chains at resonance. It is also shown that the transmission level is very sensitive to the nanoparticle environment, thu…
We have used a gold nanohole array to trap single polystyrene nanoparticles, with a mean diameter of 30 nm, into separated hot spots located at connecting nanoslot regions. A high trap stiffness of approximately 0.85 fN/(nmmW) at a low incident laser intensity of ~0.51 mW/um2 at 980 nm was obtained. The experimental results were compared to the simulated trapping force and a reasonable match was achieved. This plasmonic array is useful for lab-on-a-chip applications and has particular appeal for trapping multiple nanoparticles with predefined separations or arranged in patterns in order to stu…
Surface enhanced Raman scattering (SERS) is optically sensitive and chemically specific to detect single molecule spectroscopic signatures. Facilitating this capability in optically-trapped nanoparticles at low laser power remains a significant challenge. In this letter, we show single molecule SERS signatures in reversible assemblies of trapped plasmonic nanoparticles using a single laser excitation (633 nm). Importantly, this trap is facilitated by the thermoplasmonic field of a single gold nanoparticle dropcasted on a glass surface. We employ bi-analyte SERS technique to ascertain the singl…
The second-harmonic generation of 150 nm spherical gold nanoparticles is investigated both experimentally and theoretically. We demonstrate that the interference effects between dipolar and octupolar plasmons can be used as a fingerprint to discriminate the local surface and non-local bulk contributions to the second-harmonic generation. By fitting the experimental data with the electric fields computed with finite-element method (FEM) simulations, the Rudnick and Stern parameters weighting the relative nonlinear sources efficiencies are evaluated and the validity of the hydrodynamic model and…
Laboratoire Kastler Brossel（卡斯特勒·布罗塞尔实验室）；Ecole Normale Supérieure（巴黎高等师范学院）；UPMC（巴黎第六大学（皮埃尔和玛丽·居里大学））；Laboratoire Charles Coulomb（查尔斯·库仑实验室）；Université Montpellier II（蒙彼利埃第二大学）
In this paper we present a digital holographic microscope to track gold colloids in three dimensions. We report observations of 100nm gold particles in motion in water. The expected signal and the chosen method of reconstruction are described. We also discuss about how to implement the numerical calculation to reach real-time 3D tracking.
Here we demonstrate a novel smart magnetoplasmonic heterostructure for efficient control of light. It consists of gold nanoparticles embedded in a thin magnetic film covered with a gold layer pierces with periodic nanoslit array. Unique feature of the proposed structure is that it supports four different types of optical modes in the same frequency range including localized and propagating surface plasmons along with waveguide modes. A peculiar magneto-optical response appears at the frequencies of the mode hybridization. The most prominent result comes from hybridization of the localized and …
Mechanically interlocked molecules have marked a breakthrough in the field of topological chemistry and boosted the vigorous development of molecular machinery. As an archetypal example of the interlocked molecules, catenanes comprise macrocycles that are threaded through one another like links in a chain. Inspired by the transition metal-templated approach of catenanes synthesis, the hierarchical assembly of DNA origami catenanes templated by gold nanoparticles is demonstrated in this work. DNA origami catenanes, which contain two, three or four interlocked rings are successfully created. In …
Assemblies of closely separated gold nanoparticles exhibit a strong collective plasmonic response due to coupling of the plasmon modes of the individual nanostructures. In the context of self-assembly of nanoparticles, closed packed 2D clusters of spherical nanoparticles present an important composite system that promises numerous applications. The present study probes the collective plasmonic characteristics and resulting photothermal behavior of closed packed 2D Au nanoparticle clusters in order to delineate the effects of cluster size, inter-particle distance and particle size. Smaller nano…
The strong interaction of light with metallic nanoparticles enables field confinement well below the diffraction limit. Plasmonic waveguides consisting of metal nanoparticle chains could be used for the propagation of energy or information on the nanoscale, but high losses have thus far impeded practical applications. Here we demonstrate that efficient waveguiding is possible through gold nanoparticle chains despite the high dissipative losses of gold. A DNA origami directed self-assembly of monocrystalline, spherical nanoparticles allows the interparticle spacing to be decreased to 2 nm or be…
We developed a microscope intended to probe, using a parallel heterodyne receiver, the fluctuation spectrum of light quasi-elastically scattered by gold nanoparticles diffusing in viscous fluids. The cutoff frequencies of the recorded spectra scale up linearly with those expected from single scattering formalism in a wide range of dynamic viscosities (1 to 15 times water viscosity at room temperature). Our scheme enables ensemble-averaged optical fluctuations measurements over multispeckle recordings in low light, at temporal frequencies up to 10 kHz, with a 12 Hz framerate array detector.
Self-organized collective behaviour of active units is inspiring new designs of artificial swarms of micron-sized objects. However, active control at the nanoscale remains elusive. We have accurately solved the collective optofluidic dynamics of gold plasmonic 50 nm-radius nanoparticles moving in aqueous solution under a nonconservative optical vortex lattice. Above a critical field intensity and concentration, the interplay between optical forces, thermal fluctuations and hydrodynamic pairing leads to a spontaneous transition towards synchronised motion exhibiting a rich assortment of collect…
A nanofabricated regular array of coupled gold nano-pillars is employed to detect local indices of refraction of different liquids using a shift of an antisymmetric plasmon resonance peak observed in the reflection spectra. The peak spectral position is found to be a unique function of the local refractive index for a wide range of indices. We discuss possible applications of the fabricated nanostructured arrays in bio and chemical sensors.
We investigate plasmon resonances in gold nanoparticles to enhance the quantum yield of upconverting materials. For this purpose, we use a rate equation model that describes the upconversion of trivalent erbium based upconverters. Changes of the optical field acting on the upconverter and the changes to the transition probabilities of the upconverter in the proximity of a gold nanoparticle are calculated using Mie theory and exact electrodynamic theory respectively. With this data, the influence on the luminescence of the upconverter is determined using the rate equation model. The results sho…
Noble metal nanoparticles show specific optical properties due to the excitation of localized surface plasmons that make them attractive candidates for highly sensitive bionanosensors. The underlying physical principle is either an analyte-induced modification of the dielectric properties of the medium surrounding the nanoparticle or an increase of the excitation and emission rates of an optically active analyte by the resonantly enhanced plasmon field. Either way, besides the nanoparticle geometry the dielectric properties of the metal and nanoscale surface roughness play an important role fo…
We demonstrate stimulated emission depletion (STED) microscopy with 20 nm gold nanospheres coated by fluorescent silica. Compared with previous demonstrations of STED with a hybrid plasmonic fluorescent label, the current implementation offers a substantially smaller label and a better resolution improvement of up to 2.5-fold beyond the diffraction limit of confocal microscopy. This is achieved at approximately 2 times lower intensity than conventional STED based on dyes alone, and in an aqueous environment, demonstrating the relevance to bio-imaging. Finally, we also show, for the first time …
Tracking individual nano-objets in live cells during arbitrary long times is an ubiquitous need in modern biology. We present here a method for tracking individual 5 nm gold nanoparticles on live cells. It relies on the photothermal effect and the detection of the Laser Induced Scattering around a NanoAbsorber (LISNA). The key point for recording trajectories at video rate is the use of a triangulation procedure. The effectiveness of the method is tested against Single fluorescent Molecule Tracking in live COS7 cells on subsecond time scales. We further demonstrate recordings for several minut…
