Gold Nanodisks Research Articles

Impact of supporting nanometric membranes on the thermo-optical dynamics of individual plasmonic nanodisks.

The thermal dynamics and transient optical response of individual gold nanodisks supported on thin silicon nitride membranes were investigated using optical time-resolved pump-probe spectroscopy and finite-element modeling. The effect of reducing the membrane thickness from 50 nm to 15 nm on the nanodisk thermal dynamics was explored. A significant deceleration of the nanodisk cooling kinetics was observed, and linked to a quasi-two-dimensional heat diffusion process within the 15 nm thick membrane, without detectable modification of its thermal conductivity. Systematic measurements involving different optical probe wavelengths additionally revealed the contribution of indirect membrane heating to the measured time-resolved signals, an effect particularly pronounced in the spectral range where direct optical heating of the nanodisk induces minimal ultrafast modifications of its extinction cross-section.

Efficient monodisperse upconversion composite prepared using high-density local field and its dual-mode temperature sensing.

Enhanced upconversion via plasmonics has considerable potential in biosensors and solar cells; however, conventional plasmonic configurations such as core-shell assemblies or nanoarray platforms still suffer from the compromise between the enhancement factor and monodispersity, which has failed to meet the requirement of the materials for the in vivo all-solution-prepared solar cells and biosensors. We herein report a monodisperse metal-dielectric-metal (MDM) type upconverted hybrid material with high efficiency. The lanthanide-doped upconversion nanoparticles (UCNPs) were sandwiched by two gold nanodisk mirrors, and the highly localized excitation field around the UCNPs together with the efficient coupling enhanced the upconversion. The upconversion intensity can then be effectively regulated and improved by three to four orders of magnitude. As per the measurement of the temperature-dependent fluorescence intensity and spectra shift, a dual-mode nanothermometer based on our proposed hybrid materials was demonstrated. This MDM-type upconverted hybrid material demonstrated the merits of high efficiency and monodispersity, which demonstrated promise in in vivo biosensors and solar cell fabrication techniques such as spin-coating and roll-to-roll.

Resonant Raman scattering on graphene: SERS and gap-mode TERS.

Nanoscale deformations and corrugations occur in graphene-like two-dimensional materials during their incorporation into hybrid structures and real devices, such as sensors based on surface-enhanced Raman scattering (SERS-based sensors). The structural features mentioned above are known to affect the electronic properties of graphene, thus highly sensitive and high-resolution techniques are required to reveal and characterize arising local defects, mechanical deformations, and phase transformations. In this study, we demonstrate that gap-mode tip-enhanced Raman Scattering (gm-TERS), which offers the benefits of structural and chemical analytical methods, allows variations in the structure and mechanical state of a two-dimensional material to be probed with nanoscale spatial resolution. In this work, we demonstrate locally enhanced gm-TERS on a monolayer graphene film placed on a plasmonic substrate with specific diameter gold nanodisks. SERS measurements are employed to determine the optimal disk diameter and excitation wavelength for further realization of gm-TERS. A significant local plasmonic enhancement of the main vibrational modes in graphene by a factor of 100 and a high spatial resolution of 10 nm are achieved in the gm-TERS experiment, making gm-TERS chemical mapping possible. By analyzing the gm-TERS spectra of the graphene film in the local area of a nanodisk, the local tensile mechanical strain in graphene was detected, resulting in a split of the G mode into two components, G+ and G-. Using the frequency split in the positions of G+ and G- modes in the TERS spectra, the stress was estimated to be up to 1.5%. The results demonstrate that gap-mode TERS mapping allows rapid and precise characterization of local structural defects in two-dimensional materials on the nanoscale.

A scalable fabrication method for gold nanodisk-upconverting nanoparticle hybrid nanostructures.

Plasmonic nanostructures can be used to enhance the efficiency of upconversion nanoparticles (UCNPs) and enable new functionalities. However, the fabrication of these hybrid plasmon-UCNP nanostructures has traditionally relied on either wet chemistry or nanolithography routes that are difficult to control, scale up, or both. In this work, we present a scalable nanofabrication process, capable of producing a massive array of gold-UCNP hybrid nanostructures over a few mm2 area and with excellent uniformity in the photoluminescence intensity. This new approach combines the scalability of the bottom-up self-assembly method and the precision of the top-down nanolithography approach. It provides an efficient alternative route for the production of plasmonically enhanced UCNPs. A detailed discussion on the optimization of the UCNP self-assembly, the gold nanodisk lithography, and the nanopattern transfer processes is presented here. Additionally, we showcase the potential of this new approach for fabricating mechanical force sensors based on the selective plasmonic enhancement of the UCNP emission. This new approach holds great potential in facilitating the production of plasmonically enhanced UCNPs that can be deployed for both imaging and sensing applications.

Novel Nano-Electroplating-Based Plasmonic Platform for Giant Emission Enhancement in Monolayer Semiconductors.

Two-dimensional semiconductors such as monolayer MoS2 have attracted considerable attention owing to their exceptional electronic and optical characteristics. However, their practical application has been hindered by the limited light absorption resulting from atomically thin thickness and low quantum yield. A highly effective approach to address these limitations is by integrating subwavelength plasmonic nanostructures with monolayer semiconductors. In this study, we employed electron beam lithography and nanoelectroplating techniques to develop a gold nanodisc (AuND) array plasmonic platform. Monolayer MoS2 transferred on top of the AuND array yields up to 150-fold photoluminescence enhancement compared to a gold film without normalization with respect to plasmonic hot spots. In addition, the unique protocol of nanoelectroplating helps to get flat-top cylindrical discs which enable less tear during the delicate wet transfer of monolayer MoS2. We explain our experimental findings based on electromagnetic simulations.

Bound states in the continuum in a waveguide structure covered by a two-dimensional square array of gold nanodisks

Bound states in the continuum in a waveguide structure covered by a two-dimensional square array of gold nanodisks

Balancing detectivity and sensitivity of plasmonic sensors with surface lattice resonance

Abstract Resonators are at the core of optical sensors enhancing light–analyte interaction and leading to higher sensitivities. Maximizing the sensitivity is an obvious objective function for the resonator design. However, high sensitivity does not guarantee sufficient detectivity. When the optical energy budget is limited, as in sensors on mobile platforms, a higher sensitivity usually leads to lower detectivity for nanophotonic sensors. In such scenarios, resonator design requires balancing the trade-off between the sensitivity and detectivity of the resonant sensor. Here, we show the direct dependence of detectivity on the Q-factor and the trade-off between the Q-factor and sensitivity. We study this trade-off in an array of plasmonic resonators. We choose plasmonic resonators because of their high sensitivity arising from large local field enhancements. Then, we show that the detectivity of this sensor may be boosted for limited energy budget applications by making an array of resonators supporting a surface lattice resonance (SLR). We experimentally demonstrate sensing and detection of antimouse IgG protein in a gold nanodisk array–based SLR sensor for various energy budgets.

Efficient second harmonic generation at quasi-bound states in the continuum in hybrid nanostructures of 2D plasmonic array and waveguide

We numerically investigate the second harmonic generation (SHG) in hybrid plasmonic–photonic structures consisting of an array of periodic gold nanodisks covered by a nonlinear dielectric layer. In the designed hybrid systems, symmetry-protected bound states in the continuum (BICs) at normal incidence, and Friedrich–Wintgen BICs due to the coupling between localized surface plasmon resonances (LSPRs) and waveguide modes at oblique incidence, are observed under both transverse-electric (TE) and transverse-magnetic (TM) polarized illuminations. SHG near the BICs is studied, and the dramatically enhanced nonlinear optical response at quasi-BICs is obtained. Such enhancement is ascribed to the enhanced local field due to hybrid modes of LSPRs and photonic modes. The results indicate that hybrid plasmonic-dielectric systems supporting BICs at both TE- and TM-polarized incidences are promising platforms for linear and nonlinear photonic devices.

Designing optical hyperbolic metasurfaces based on gold nanodisks

Hyperbolic metasurfaces (HMSs) have demonstrated great value for planar and near-field applications. Nevertheless, the ability to engineer a specific HMS design with predefined functionality is still a challenge. Here, we study dozens of HMSs based on gold nanodisks in the visible spectrum and analyze their properties. In particular, we connect the geometric configuration of a metasurface with its spectral hyperbolicity bandwidth and the efficiency of hyperbolic plasmon-polariton canalization. We also analyze the impact of the substrate on the hyperbolic regime of a metasurface. As a result, we derive a universal empirical formula allowing us to obtain the approximate design of a HMS immediately. We provide practical guidelines for designing HMSs that may be used for a plethora of photonic applications.

Imaging and Controlling Ultrafast Electron Pulses Emitted from Plasmonic Nanostructures.

We experimentally study photoemission from gold nanodisk arrays using space-, time-, and energy-resolved photoemission electron microscopy. When excited by a plasmonic resonant infrared (IR) laser pulse, plasmonic hotspots are generated owing to local surface plasmon resonance. Photoelectrons emitted from each plasmonic hotspot form a nanoscale and ultrashort electron pulse. When the system is excited by an extreme ultraviolet (EUV) laser pulse, a uniformly distributed photoelectron cloud is formed across the sample surface. When excited by the IR and EUV laser pulses together, both the photoemission image and kinetic energy vary significantly for the IR laser-generated electrons depending on the time delay between the two laser pulses. These observations are well explained by the Coulomb interaction with the EUV laser-generated electron cloud. Our study offers a feasible approach to manipulate the energy of electron pulse emitted from a plasmonic nanostructure on an ultrafast time scale.

Metasurface for broadband coherent Raman signal enhancement beyond the single-molecule detection threshold

Broadband enhancement of Raman signals is vital for molecular spectroscopy and sensing applications. However, typically, there is a compromise between the resonance width and the local field enhancement factors. Here, we merge the broadband open plasmonic cavity concepts with the geometry exploiting narrow gaps and a reflecting layer. This results in a metasurface design that maintains substantial electric field confinement in the gap volume accompanied by a broad spectral response. The confined field is enhanced through constructive interference between the plasmonically enhanced illuminating beam and the field reflected at the bottom layer. The resulting field can interact with analyte molecules and support Raman scattering. With an optimized metasurface geometry involving a pair of gold nanodisks and a thin gold film, we demonstrate numerically that our metasurface can simultaneously enhance Raman signals from various molecular species, potentially resulting in unprecedented signal intensities enhanced by up to 20 orders of magnitude, facilitating molecular detection and identification. Our design offers a practical and promising solution for improving the sensitivity of Raman techniques and has significant implications for the field of nonlinear optical spectroscopy. Moreover, our metasurface is compatible with current fabrication technologies, making it suitable for various applications in sensing and imaging.

Single-Exosome Counting and 3D, Subdiffraction Limit Localization Using Dynamic Plasmonic Nanoaperture Label-Free Imaging.

Blood-circulating exosomes as a disease biomarker have great potential in clinical applications as they contain molecular information about their parental cells. However, label-free characterization of exosomes is challenging due to their small size. Without labeling, exosomes are virtually indistinguishable from other entities of similar size. Over recent years, several techniques have been developed to overcome the existing challenges. This paper demonstrates a new label-free approach based on dynamic PlAsmonic NanO-apeRture lAbel-free iMAging (D-PANORAMA), a bright-field technique implemented on arrayed gold nanodisks on invisible substrates (AGNIS). PANORAMA provides high surface sensitivity and has been shown to count single 25 nm polystyrene beads (PSB) previously. Herein, we show that using the dynamic imaging mode, D-PANORAMA can yield 3-dimensional, sub-diffraction limited localization of individual 25 nm beads. Furthermore, we demonstrate D-PANORAMA's capability to size, count, and localize the 3-dimensional, sub-diffraction limited position of individual exosomes as they bind to the AGNIS surface. We emphasize the importance of both the in-plane and out-of-plane localization, which exploit the synergy of 2-dimensional imaging and the intensity contrast.

High gain hot-carrier WSe2 phototransistor with gate-tunable responsivity

Hot-carrier injection at semiconductor/metal interface shows great potentials in infrared photodetection. However, the photoresponsivity of hot-carrier photodetector with diode mode is still limited in the scale of 1 mA/W due to the low injection efficiency of hot carriers and the lack of gain. Here, we demonstrate a high gain hot-carrier WSe2 phototransistor with gate-tunable responsivity. In this device, plasmonic resonances is used to enhance the light absorption of gold nanodisk, which provide hot holes. The hot holes are trapped into WSe2 and recycled in WSe2 channel in lateral direction, which introduce high gain for photodetection. Experiment shows that the photoresponsivity of the device can be over 0.23 A/W with a gain of 270 at the wavelength of 1310 nm. More interestingly, the responsivity of the device can be tuned by gate, which can be used to encode synaptic weights of the sensor pixel.

Engineering Substrate-Mediated Localized Surface Plasmons in Gold Nanodiscs

A variety of nanostructures capable of generating strong local electromagnetic fields (hot spots) in interaction with radiation have been under intensive investigation towards plasmonic applications in surface-enhanced Raman scattering (SERS), biosensing, broadband absorbers, thermophotovoltaics, photocatalysis, etc. In many cases, these nanostructures are formed on a surface or embedded into a near-surface layer of the dielectric substrate, making some part of the field dissipate into the bulk and not contribute to the desired plasmonic functionality. To reduce such losses, the interface between the metallic nanostructures and the dielectric environment should be engineered. In the current work, Au nanodiscs are fabricated on Si posts of very small diameter (pin-shaped structures), enabling them to decouple the strong optical near fields localized at the nanodiscs from the bulk Si substrate. The Si post diameter is optimized by adjusting the gas flow rates in reactive-ion etching, resulting in a minimum post diameter of 20 nm at the nanodisc interface. The effect of this diameter on the localized surface plasmon resonance of the nanodisc is investigated with linear optical spectroscopic measurements, where a significant spectral blue shift of the resonance band is noticed compared to similar discs formed on bulk Si surface. The experimental results are compared with modelling where a 3-fold increase in the electric field enhancement is demonstrated. The fabricated pin-shaped nanostructures are tested in SERS measurements showing a significant increase in the enhancement factor in the order of 106. Thus, this work suggests a way of engineering 3D morphology to tune the substrate influence on the plasmonic properties of nanostructures and to develop efficient nanofabrication technologies.

Cooling Dynamics of Individual Gold Nanodisks Deposited on Thick Substrates and Nanometric Membranes.

The cooling dynamics of individual gold nanodisks synthesized using colloidal chemistry and deposited on solid substrates with different compositions and thicknesses were investigated using optical time-resolved spectroscopy and finite-element modeling. Experiments demonstrate a strong substrate-dependence of these cooling dynamics, which require the combination of heat transfer at the nanodisk/substrate interface and heat diffusion in the substrate. In the case of nanodisks deposited on a thick sapphire substrate, the dynamics are found to be mostly limited by the thermal resistance of the gold/sapphire interface, for which a value similar to that obtained in the context of previous experiments on sapphire-supported single gold nanodisks produced by electron beam lithography is deduced. In contrast, the cooling dynamics of nanodisks supported by nanometric silica and silicon nitride membranes are much slower and largely affected by heat diffusion in the membranes, whose efficiency is strongly reduced as compared to the thick sapphire case.

Synthesis of Metal/SU-8 Nanocomposites through Photoreduction on SU-8 Substrates.

The paper presents a simple, fast, and cost-effective method for creating metal/SU-8 nanocomposites by applying a metal precursor drop onto the surface or nanostructure of SU-8 and exposing it to UV light. No pre-mixing of the metal precursor with the SU-8 polymer or pre-synthesis of metal nanoparticles is required. A TEM analysis was conducted to confirm the composition and depth distribution of the silver nanoparticles, which penetrate the SU-8 film and uniformly form the Ag/SU-8 nanocomposites. The antibacterial properties of the nanocomposites were evaluated. Moreover, a composite surface with a top layer of gold nanodisks and a bottom layer of Ag/SU-8 nanocomposites was produced using the same photoreduction process with gold and silver precursors, respectively. The reduction parameters can be manipulated to customize the color and spectrum of various composite surfaces.

Multiphysics Modeling of Plasmon-Enhanced All-Optical Helicity-Dependent Switching.

In this work, we propose a multiphysics approach to simulate all-optical helicity-dependent switching induced by the local hot spots of plasmonic nanostructures. Due to the plasmonic resonance of an array of gold nanodisks, strong electromagnetic fields are generated within the magnetic recording media underneath the gold nanodisks. We construct a multiphysics framework considering the opto-magnetic and opto-thermal effects, and then model the magnetization switching using the Monte Carlo method. Our approach bridges the gap between plasmonic nanostructure design and magnetization switching modeling, allowing for the simulation of helicity-dependent, nanoscale magnetization switching in the presence of localized surface plasmons.

Plasmonic Resonance Coupling of Nanodisk Array/Thin Film on the Optical Fiber Tip for Integrated and Miniaturized Sensing Detection.

Fiber-optic surface plasmon resonance (FOSPR) sensing technology has become an appealing candidate in biochemical sensing applications due to its distinguished capability of remote and point-of-care detection. However, FOSPR sensing devices with a flat plasmonic film on the optical fiber tip are seldom proposed with most reports concentrating on fiber sidewalls. In this paper, we propose and experimentally demonstrate the plasmonic coupled structure of a gold (Au) nanodisk array and a thin film integrated into the fiber facet, enabling the excitation of the plasmon mode on the planar gold film by strong coupling. This plasmonic fiber sensor is fabricated by the ultraviolet (UV) curing adhesive transferring technology from a planar substrate to a fiber facet. The experimental results demonstrate that the fabricated sensing probe has a bulk refractive index sensitivity of 137.28 nm/RIU and exhibits moderate surface sensitivity by measuring the spatial localization of its excited plasmon mode on Au film by layer-by-layer self-assembly technology. Furthermore, the fabricated plasmonic sensing probe enables the detection of bovine serum albumin (BSA) biomolecule with a detection limit of 19.35 μM. The demonstrated fiber probe here provides a potential strategy to integrate plasmonic nanostructure on the fiber facet with excellent sensing performance, which has a unique application prospect in the detection of remote, in situ, and in vivo invasion.

2D Assembly of Atomically Oriented Gold Nanodisks Leads to Tunable Plasmonic Resonance

2D Assembly of Atomically Oriented Gold Nanodisks Leads to Tunable Plasmonic Resonance

Photon superbunching in cathodoluminescence of excitons in WS2 monolayer

Cathodoluminescence spectroscopy in conjunction with second-order auto-correlation measurements of allows to extensively study the synchronization of photon emitters in low-dimensional structures. Co-existing excitons in two-dimensional transition metal dichalcogenide monolayers provide a great source of identical photon emitters which can be simultaneously excited by an electron. Here, we demonstrate large photon bunching with up to of a tungsten disulfide monolayer (WS2), exhibiting a strong dependence on the electron-beam current. To further improve the excitation synchronization and the electron-emitter interaction, we show exemplary that the careful selection of a simple and compact geometry—a thin, monocrystalline gold nanodisk—can be used to realize a record-high bunching of up to . This approach to control the electron excitation of excitons in a WS2 monolayer allows for the synchronization of photon emitters in an ensemble, which is important to further advance light information and computing technologies.