Gold Nanodisks Research Articles

Coherent Acoustic Phonons in Plasmonic Nanoparticles: Elastic Properties and Dissipation at Low Temperatures.

We studied the frequency and quality factor of mechanical plasmonic nanoresonators as a function of temperature, ranging from ambient to 4 K. Our investigation focused on individual gold nanorods and nanodisks of various sizes. We observed that oscillation frequencies increase linearly as temperature decreases until saturation is reached at cryogenic temperatures. This behavior is explained by the temperature dependence of the elastic modulus, with a Debye temperature compatible with reported bulk values for gold. To describe the behavior of the quality factor, we developed a model considering the nanostructures as anelastic solids, identifying a dissipation peak around 150 K due to a thermally activated process, likely of the Niblett-Wilks mechanism type. Importantly, our findings suggest that external dissipation factors are more critical to improving quality factors than internal friction, which can be increased by modifying the nanoresonator's environment. Our results enable the future design of structures with high vibration frequencies and quality factors by effectively controlling external losses.

Active infrared tuning of metal–insulator-metal resonances by VO2 thin film

VO2 is a promising phase change material offering a large contrast of electric, thermal, and optical properties when transitioning from semiconductor to metallic phase. Here we show that a hybrid metamaterial obtained by proper combination of a VO2 layer and a nanodisk gold array provides a tunable plasmonic gap resonance in the infrared range. Specifically, we have designed and fabricated a metal–insulator-metal gap resonance by inserting sub-wavelength VO2 film between a flat gold layer and a gold nanodisk resonator array. The resonance of the hybrid metamaterial is centered in the useful 3–5 μm range when VO2 is in its semiconductor state. The experimental study highlights a monotonical spectral tuning of the resonance when increasing temperature up to 50 °C above the room temperature, providing a continuous resonance shift of almost 1 μm in the mid-infrared range. Wavelength range and intensity tunability can be further optimized by modifying the thicknesses of the layers and metamaterial parameters.

Plasmonic Coupling for High‐Sensitivity Detection of Low Molecular Weight Molecules

This article presents a novel plasmonic sensing platform designed for the detection of low molecular weight molecules, offering significant advancements in diagnostic applications. The platform features a periodic array of gold nanodisks on a 20 nm thin silica layer, supported by a 100 nm thick gold substrate. By leveraging the coupling between localized and propagating surface plasmon resonances, this design significantly enhances the sensitivity and specificity of molecular detection. Finite element method simulations are conducted to characterize the optical properties and reflectance response of the nanodisks array in the visible to near‐infrared range. Ellipsometric analysis is performed to measure the reflectance of the sample at various angles. Additionally, scanning near‐field optical microscopy in reflectance mode validates the design by revealing well‐defined plasmonic hot spots and interference patterns consistent with the simulated results. The findings demonstrate the platform's effectiveness in amplifying optical signals, achieving a limit of detection of 50 μM for molecules with a molecular weight of less than 1 KDa. This high sensitivity and specificity highlight the potential of the proposed plasmonic platform to advance the development of highly sensitive sensors for low molecular weight molecules, making it a valuable tool for diagnostics and precise molecular detection.

Plasmonic enhancement of Faraday rotation with gold nanodisks with low height-to-diameter aspect ratios

We investigate the Faraday rotation induced in gold nanodisks with low height-to-diameter aspect ratios. Through a systematic study, we analyze the phenomenon using electrostatic theory with the modified long-wavelength approximation. We show that the Faraday rotation is enhanced at the localized surface plasmon resonance when the nanodisk’s effective mean free path is equal to the mean free path of the conduction electrons in the bulk metal, where light absorption dominates over light scattering. We also show that the Faraday rotation is largely enhanced at shorter rather than longer wavelengths.

Improving the color gamut of gold nanostructures using vertical tandem nano-disks

Metallic nanoparticles have been used in structural coloration applications since they provide an alternative for the synthesis of color filters, with extended color gamut, enhanced color saturation, and brightness. These optical properties can be further improved when integrating nanoparticles into coupled dimers that give rise to enhanced hybridized plasmon resonances. In this contribution, gold nano-disks are split into Au/SiO2/Au layered structures to enhance its plasmon resonances and evaluate its improved performance as reflective color filters. To do so, the reflectance spectra of the layered disks were obtained with numerical simulations, identifying high amplitude peaks in the visible band and low-amplitude peaks in the near infrared one, related to the hybridized resonances. By choosing the appropriate size of the intermediate dielectric and metallic layers, as well as the near-field coupling, peaks can be tuned along the visible and near infrared bands, respectively. The chromatic coordinates of the addressed nanostructures obtained from the reflectance spectra show that the nanostructures hold color gamut that extends toward magenta, orange, yellowish, and reddish shades of colors.

Increasing the electric field amplification in the metal-insulator-metal structure with a grating hybrid of bowtie nanotriangle and cylindrical nanodisc

In this paper, the strong electromagnetic coupling between an integrated grating of an array of periodic gold nanodiscs and an array of bowtie nanotriangles placed on layers of a dielectric and a metal has been investigated. The upper layer is periodically created by removing each nanodisk in the array of nanodisks and replacing it with bowtie nanotriangles. The structure for near field radiation with linear polarization at 800nm wavelength is optimized so that it has the highest amount of amplification in the gap space between the tips of the nanotriangle with a minimum value of 188 times and a maximum of 320 times. The simulation results confirm that the huge field enhancement obtained is due to the strong coupling between the LSPR formed in the grating of bowties nano triangle and nanodiscs and the SPPs formed in the metal film. The amount of amplification compared to the array of only nanodiscs (about 32 times) or only bowtie nano triangles (about 120 times) is not only higher, but also the anti-crossing behavior is observed. The high amplification obtained at the mentioned wavelength can be used for laser oscillators with a central wavelength of 800nm, such as titanium sapphire, etc., which has many applications in near-field physics, SERS, and ultrafast lasers.

(Invited) Plasmonic Nanofabrication of Chiral Nanodisk Ensembles

Chiral plasmonic nanostructures attract attention because those could be applied to enantioselective chemical sensors, optical isolators, light sources for circularly polarized light (CPL), metasurfaces, and metamaterials. In many cases, chiral plasmonic nanostructures are fabricated by a top-down method such as electron beam lithography (EBL). Since EBL is time-consuming and expensive, we have developed photoelectrochemical methods in which a site-selective reaction is driven by optical near field generated around anisotropic metal nanoparticles under right- or left-CPL. As anisotropic metal precursors for preparation of chiral nanoparticles, we have used gold or silver nanocuboids, nanorods, nanocubes, and triangular or hexagonal nanoplates so far.1-5 In the present work we demonstrate that laterally isotopic, circular nanodisks can also be used as precursors for the preparation of chiral nanostructures.We prepared ensembles of circular gold nanodisks on a glass plate by a nanosphere lithography method. A glass plate was coated with a gold thin film, and an array of polystyrene spheres (500 nm diameter) was prepared on the gold film. The polystyrene spheres were etched by oxygen plasma, and the exposed gold film was etched by argon ion milling. As a result, an ensemble of gold nanodisks (~200 nm diameter) was obtained. Each nanodisk was capped with a polystyrene cone, and the cap was removed by sonication in toluene if necessary. We used both capped and uncapped nanodisk ensembles. The ensemble was irradiated with visible right- or left-CPL in the presence of silver ions and sodium citrate. The obtained Au-Ag nanostructures exhibited circular dichroism (CPL), indicating that the nanostructures have chirality. Initial deposition at arbitrary site may break the geometric symmetry, resulting in the growth into chiral structures. Saito, K.; Tatsuma, T. Nano Lett. 2018, 18, 3209–3212.Morisawa, K.; Ishida, T.; Tatsuma, T. ACS Nano 2020, 14, 3603–3609.Shimomura, K.; Nakane, Y.; Ishida, T.; Tatsuma, T. Appl. Phys. Lett. 2023, 122, 151109.Homma, T.; Sawada, N.; Ishida, T.; Tatsuma, T. ChemNanoMat 2023, 9, e202300096.Ishida, T.; Isawa, A.; Kuroki, S.; Kameoka, Y.; Tatsuma, T. Appl. Phys. Lett. 2023, 123, 061111.

Metasurface of Strongly Coupled Excitons and Nanoplasmonic Arrays.

Metasurfaces allow light to be manipulated at the nanoscale. Integrating metasurfaces with transition metal dichalcogenide monolayers provides additional functionality to ultrathin optics, including tunable optical properties with enhanced light-matter interactions. In this work, we demonstrate the realization of a polaritonic metasurface utilizing the sizable light-matter coupling of excitons in monolayer WSe2 and the collective lattice resonances of nanoplasmonic gold arrays. We developed a novel fabrication method to integrate gold nanodisk arrays in hexagonal boron nitride and thus simultaneously ensure spectrally narrow exciton transitions and their immediate proximity to the near-field of array surface lattice resonances. In the regime of strong light-matter coupling, the resulting van der Waals metasurface exhibits all key characteristics of lattice polaritons, with a directional and linearly polarized far-field emission profile dictated by the underlying nanoplasmonic lattice. Our work can be straightforwardly adapted to other lattice geometries, establishing structured van der Waals metasurfaces as means to engineer polaritonic lattices.

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.

Simplifying asynchronous optical sampling: an experimental approach toward industrial integration exploiting lock-in acquisition

Time-resolved optical spectroscopies are emerging as a go-to technique for non-destructive testing of nanomaterials. Inspecting the thermal and mechanical properties of a mesoscale device requires achieving delay times beyond the ns timescale in a nanoscopy setup, potentially in a vibration polluted environment. These requirements constitute a major challenge for traditional pump-probe techniques based on moving mechanical delay lines and lock-in detection. Asynchronous optical sampling (ASOPS) and electronically controlled optical sampling (ECOPS), avoiding any moving mechanical parts, are good alternatives. However, their detection scheme is based on fast-balanced photodiodes, which, as a technology, are not as widespread, not as developed, and lack the performance of lock-in based detection. In this study, we introduce what we believe is a novel approach that integrates ASOPS/ECOPS and lock-in detection methodologies, eliminating the necessity for a reference signal and streamlining the optical configuration. By leveraging the strengths of each technique, our approach enhances simplicity and efficiency. The scheme is first validated against standard approaches in the frame of a beam-depletion measurement in a sum frequency experiment. It is then tested in a paradigmatic case study to inspect the mechanics of a single gold nanodisk, with dimensions in the 100 nm range, nanopatterned on a sapphire substrate. These results widen the range of applicability of time-resolved optical techniques as a nano-metrology tool to industrial settings.

A novel biomimetic nanoplasmonic sensor for rapid and accurate evaluation of checkpoint inhibitor immunotherapy.

Immune checkpoint inhibitors (ICIs) emerged as promising immunotherapies for cancer treatment, harnessing the patient's immune system to fight and eliminate tumor cells. However, despite their potential and proven efficacies, checkpoint inhibitors still face important challenges such as the tumor heterogeneity and resistance mechanisms, and the complex in vitro testing, which limits their widespread applicability and implementation to treat cancer. To address these challenges, we propose a novel analytical technique utilizing biomimetic label-free nanoplasmonic biosensors for rapid and reliable screening and evaluation of checkpoint inhibitors. We have designed and fabricated a low-density nanostructured plasmonic sensor based on gold nanodisks that enables the direct formation of a functional supported lipid bilayer, which acts as an artificial cell membrane for tumor ligand immobilization. With this biomimetic scaffold, our biosensing approach provides real-time, highly sensitive analysis of immune checkpoint pathways and direct assessment of the blocking effects of monoclonal antibodies in less than 20min/test. We demonstrate the accuracy of our biomimetic sensor for the study of the programmed cell death protein 1 (PD1) checkpoint pathway, achieving a limit of detection of 6.7ng/mL for direct PD1/PD-L1 interaction monitoring. Besides, we have performed dose-response inhibition curves for an anti-PD1 monoclonal antibody, obtaining a half maximal inhibitory concentration (IC50) of 0.43nM, within the same range than those obtained with conventional techniques. Our biomimetic sensor platform combines the potential of plasmonic technologies for rapid label-free analysis with the reliability of cell-based assay in terms of ligand mobility. The biosensor is integrated in a compact user-friendly device for the straightforward implementation in biomedical and pharmaceutical laboratories.

Plasmon‐Enhanced Optical Control of Magnetism at the Nanoscale via the Inverse Faraday Effect

The relationship between magnetization and light has been the subject of intensive research for the past century. Herein, the impact of magnetization on light polarization is well understood. Conversely, the manipulation of magnetism with polarized light is being investigated to achieve all‐optical control of magnetism, driven by potential technological implementation in spintronics. Remarkable discoveries, such as the single‐pulse all‐optical switching of magnetization in thin films and submicrometer structures, have been reported. However, the demonstration of local optical control of magnetism at the nanoscale has remained elusive. Herein, it is demonstrated that exciting gold nanodiscs with circularly polarized femtosecond laser pulses lead to ultrafast, local, and deterministic control of magnetization in an adjacent magnetic film. This control is achieved by exploiting the magnetic moment generated in plasmonic nanodiscs through the inverse Faraday effect. The results pave the way for light‐driven control in nanoscale spintronic devices and provide important insights into the generation of magnetic fields in plasmonic nanostructures.

Optical force sensor based on plasmon modulated upconversion luminescence.

We report a novel force sensor exploiting the interaction between plasmonic nanostructures and upconversion nanoparticles (UCNPs). The nanosensor is composed of a gold nanodisk and UCNPs separated by a flexible polymer layer. The gold nanodisk is designed to exhibit a plasmon resonance that selectively enhances one of the emission bands of the UCNPs while leaving the other ones largely unaffected. As the nanosensor is compressed or stretched by an external force, the polymer layer thickness changes, modulating the plasmon-UCNP coupling. The resulting changes in the luminescence intensity provides the basis for sensing. Furthermore, the nanosensor employs ratiometric sensing which makes it highly robust against any environmental variations. Our nanosensors exhibit two orders of magnitude higher responsivity than previously reported UCNP-based force sensors. They can be prepared as an on-chip sensor array or in a colloidal solution, making them suitable for a variety of applications in biology and robotics.

Focusing Surface Acoustic Waves with a Plasmonic Hypersonic Lens.

Plasmonic nanoantennas have proven to be efficient transducers of electromagnetic to mechanical energy and vice versa. The sudden thermal expansion of these structures after an ultrafast optical pulsed excitation leads to the emission of hypersonic acoustic waves to the supporting substrate, which can be detected by another antenna that acts as a high-sensitivity mechanical probe due to the strong modulation of its optical response. Here, we propose and experimentally demonstrate a nanoscale acoustic lens comprised of 11 gold nanodisks whose collective oscillation at gigahertz frequencies gives rise to an interference pattern that results in a diffraction-limited surface acoustic beam of about 340 nm width, with an amplitude contrast of 60%. Via spatially decoupled pump-probe experiments, we were able to map the radiated acoustic energy in the proximity of the focal area, obtaining a very good agreement with the continuum elastic theory.

Effect of thermal annealing on the surface plasmon properties of gold and silver nanodisk structures fabricated by electron beam lithography

This study investigates the effect of thermal annealing on the surface plasmon resonance properties of gold and silver nanodisk structures fabricated by electron beam lithography. Despite no significant size change due to a nickel adhesion layer, thermal annealing at 500 °C notably altered surface plasmon resonance properties, especially in gold nanodisks, which showed peak blue-shifts and narrowing, indicating improved crystallinity. We fitted the peak shift by using an electromagnetic field analysis and discussed the changes in the dielectric function. The dielectric function of the simple Drude model was adopted, which was fitted to the values of the Lorentz Drude model in a limited wavelength region. While both silver and gold exhibited increased oscillation strength, only gold nanodisk structures showed a decrease in damping frequency. Increased oscillation strength indicated that these structures should be useful for selective enhancement of the light at specific wavelengths by a very simple heat treatment.

Tuning the plasmonic response of periodic gold nanodisk arrays for urea sensing

Tuning the plasmonic response of periodic gold nanodisk arrays for urea sensing

Period induced reflectance tuning in transparent gold metasurfaces

Gold (Au) nanodisk arrays are modeled and fabricated for tunable near infrared reflectance with high visible transmittance. Simulations are performed in the visible and near infrared regimes between 400 and 2000 nm with varying period of nanostructures. A progressive increase in period of up to three times the diameter of the nanodisks on polymer and quartz substrates is presented. As a result, an increase in visible transmittance with a decrease in near infrared reflectance peak intensity is observed. Modeling results exhibit a high average visible transmittance of 91.5% (400–700 nm) and average reflectance of 62.9% (750–2000 nm) with diameter (D) variations from D=120 nm to D=500 nm with a period (P) equal to twice the diameter, P=2D for a polymer substrate. Electric field intensities exhibit an increase with a decrease in the period between individual nanostructures for constant unit cell dimensions. Alongside simulations, electron beam lithography and evaporation processes are utilized for the patterning and fabrication. Optical characterizations including scanning electron microscopy (SEM) and atomic force microscopy (AFM) of selected metasurfaces on quartz are performed. For a specific period and diameter, the fabricated metasurfaces exhibit near infrared reflectance having a good agreement with the simulated results about plasmonic wavelengths. Such metasurfaces offer potential to be deployed for applications that require selective reflectance intensities in the near infrared range with high visible transmittance, such as controlled environment agriculture (CEA) or multi spectral near infrared sensing. With tunability over a broadband (750–2500 nm), this simple and fabrication-friendly model may be used as a theoretical guide in quantifying specific design parameters with varying light intensity configurations.

Amplifying Sensing Capabilities: Combining Plasmonic Resonances and Fresnel Reflections through Multivariate Analysis.

Multivariate analysis applied in biosensing greatly improves analytical performance by extracting relevant information or bypassing confounding factors such as nonlinear responses or experimental errors and noise. Plasmonic sensors based on various light coupling mechanisms have shown impressive performance in biosensing by detecting dielectric changes with high sensitivity. In this study, gold nanodiscs are used as metasurface in a Kretschmann setup, and a variety of features from the reflectance curve are used by machine learning to improve sensing performance. The nanostructures of the metasurface generate new plasmonic features, apart from the typical resonance that occurs in the classical Kretschmann mode of a gold thin film, related to the evanescent field beyond total internal reflection. When the engineered metasurface is integrated into a microfluidic chamber, the device provides additional spectral features generated by Fresnel reflections at all dielectric interfaces. The increased number of features results in greatly improved detection. Here, multivariate analysis enhances analytical sensitivity and sensor resolution by 200% and more than 20%, respectively, and reduces prediction errors by almost 40% compared to a standard plasmonic sensor. The combination of plasmonic metasurfaces and Fresnel reflections thus offers the possibility of improving sensing capabilities even in commonly available setups.

Enhanced inverse Faraday effect and time-dependent thermo-transmission in gold nanodisks

Abstract Nonmagnetic media can be magnetized by light via processes referred to as an inverse Faraday effect (IFE). With nonmagnetic metal nanostructures, the IFE is dominated by the presence of light-induced solenoidal surface currents or plasmons with orbital angular momenta, whose properties depend on both the light and nanostructure geometry. Here, through a systematic study of gold nanodisks with different sizes, we demonstrate order-of-magnitude enhancement of the IFE compared to a bare gold film. Large IFE signals occur when light excites the dipolar plasmonic resonance of the gold nanodisk. We observe that the spectral response of the IFE signal mirrors the spectral response of time-dependent thermo-transmission signals. Our careful quantitative experimental measurements and analysis offer insight into the magnitude of IFE in plasmonic structures for compact, low-power, magneto-optic applications.

Twisted epitaxy of gold nanodisks grown between twisted substrate layers of molybdenum disulfide.

We expand the concept of epitaxy to a regime of "twisted epitaxy" with the epilayer crystal orientation between two substrates influenced by their relative orientation. We annealed nanometer-thick gold (Au) nanoparticles between two substrates of exfoliated hexagonal molybdenum disulfide (MoS2) with varying orientation of their basal planes with a mutual twist angle ranging from 0° to 60°. Transmission electron microscopy studies show that Au aligns midway between the top and bottom MoS2 when the twist angle of the bilayer is small (<~7°). For larger twist angles, Au has only a small misorientation with the bottom MoS2 that varies approximately sinusoidally with twist angle of the bilayer MoS2. Four-dimensional scanning transmission electron microscopy analysis further reveals a periodic strain variation (<|±0.5%|) in the Au nanodisks associated with the twisted epitaxy, consistent with the Moiré registry of the two MoS2 twisted layers.