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Infrared plasmonics: STEM-EELS characterization of Fabry-Pérot resonance damping in gold nanowires
Materials possessing strong midinfrared responses are of current interest because of their potential application to long-wavelength metamaterials, photonic devices, molecular detection, and catalysis. In this work, we utilize high-energy resolution (80 cm -1 , 10 meV) electron-energy-loss spectroscopy (EELS) in a monochromated and aberration-corrected scanning transmission electron microscope (STEM) to resolve multipolar surface plasmon resonances (SPRs), sometimes called Fabry-Pérot (FP) resonances, in gold nanowires with mode energies spanning from ~1000 to 8000 cm -1 . STEM-EELS provides access to these mid- to near-IR responses in a single acquisition, avoiding the difficulties inherent in obtaining the same data using near-field optical techniques. The experimentally measured FP resonance energies and linewidths, together with analytical modeling and full-wave numerical electrodynamics simulations, provide a comprehensive picture of the radiative and intrinsic contributions to the total damping rates. We find some FP modes with dephasing times >60fs, which is almost twice the longest previously reported plasmon dephasing time for individual Au nanoparticles in the infrared. The long dephasing times and the broad tunability of the FP resonance energies throughout the infrared region suggest additional opportunities for harnessing infrared plasmonic energy before dephasing occurs.
Coupling between plasmonic and photonic crystal modes in suspended three-dimensional meta-films
A complementary metal oxide semiconductor (CMOS) compatible fabrication method for creating three-dimensional (3D) meta-films is presented. In contrast to metasurfaces, meta-films possess structural variation throughout the thickness of the film and can possess a sub-wavelength scale structure in all three dimensions. Here we use this approach to create 2D arrays of cubic silicon nitride unit cells with plasmonic inclusions of elliptical metallic disks in horizontal and vertical orientations with lateral array-dimensions on the order of millimeters. Fourier transform infrared (FTIR) spectroscopy is used to measure the infrared transmission of meta-films with either horizontally or vertically oriented ellipses with varying eccentricity. Shape effects due to the ellipse eccentricity, as well as localized surface plasmon resonance (LSPR) effects due to the effective plasmonic wavelength are observed in the scattering response. The structures were modeled using rigorous coupled wave analysis (RCWA), finite difference time domain (Lumerical), and frequency domain finite element (COMSOL). The silicon nitride support structure possesses a complex in-plane photonic crystal slab band structure due to the periodicity of the unit cells. We show that adjustments to the physical dimensions of the ellipses can be used to control the coupling to this band structure. The horizontally oriented ellipses show narrow, distinct plasmonic resonances while the vertically oriented ellipses possess broader resonances, with lower overall transmission amplitude for a given ellipse geometry. We attribute this difference in resonance behavior to retardation effects. The ability to couple photonic slab modes with plasmonic inclusions enables a richer space of optical functionality for design of metamaterial-inspired optical components.
Localized Plasmonic Heating for Single-Molecule DNA Rupture Measurements in Optical Tweezers
To date, studies on the thermodynamic and kinetic processes that underlie biological function and nanomachine actuation in biological- and biology-inspired molecular constructs have primarily focused on photothermal heating of ensemble systems, highlighting the need for probes that are localized within the molecular construct and capable of resolving single-molecule response. Here we present an experimental demonstration of wavelength-selective, localized heating at the single-molecule level using the surface plasmon resonance of a 15 nm gold nanoparticle (AuNP). Our approach is compatible with force-spectroscopy measurements and can be applied to studies of the single-molecule thermodynamic properties of DNA origami nanomachines as well as biomolecular complexes. We further demonstrate wavelength selectivity and establish the temperature dependence of the reaction coordinate for base-pair disruption in the shear-rupture geometry, demonstrating the utility and flexibility of this approach for both fundamental studies of local (nanometer-scale) temperature gradients and rapid and multiplexed nanomachine actuation.
Structural and functional insights into the interaction between the bacteriophage T4 DNA processing proteins gp32 and Dda
Abstract Bacteriophage T4 is a classic model system for studying the mechanisms of DNA processing. A key protein in T4 DNA processing is the gp32 single-stranded DNA-binding protein. gp32 has two key functions: it binds cooperatively to single-stranded DNA (ssDNA) to protect it from nucleases and remove regions of secondary structure, and it recruits proteins to initiate DNA processes including replication and repair. Dda is a T4 helicase recruited by gp32, and we purified and crystallized a gp32–Dda–ssDNA complex. The low-resolution structure revealed how the C-terminus of gp32 engages Dda. Analytical ultracentrifugation analyses were consistent with the crystal structure. An optimal Dda binding peptide from the gp32 C-terminus was identified using surface plasmon resonance. The crystal structure of the Dda–peptide complex was consistent with the corresponding interaction in the gp32–Dda–ssDNA structure. A Dda-dependent DNA unwinding assay supported the structural conclusions and confirmed that the bound gp32 sequesters the ssDNA generated by Dda. The structure of the gp32–Dda–ssDNA complex, together with the known structure of the gp32 body, reveals the entire ssDNA binding surface of gp32. gp32–Dda–ssDNA complexes in the crystal are connected by the N-terminal region of one gp32 binding to an adjacent gp32, and this provides key insights into this interaction.
Geometrically Tunable Beamed Light Emission from a Quantum‐Dot Ensemble Near a Gradient Metasurface
Abstract Optical metasurfaces have been widely investigated in recent years as a means to tailor the wavefronts of externally incident light for passive device applications. At the same time, their use in active optoelectronic devices such as light emitters is far less established. This work explores their ability to control the radiation properties of a nearby continuous ensemble of randomly oriented incoherent dipole sources via near‐field interactions. Specifically, a film of colloidal quantum dots is deposited on a plasmonic metasurface consisting of a 1D array of metallic nanoantennas on a metal film. The array is designed to introduce a linear phase profile upon reflection, and a bi‐periodic nanoparticle arrangement is introduced to ensure adequate sampling of the desired phase gradient. Highly directional radiation patterns are correspondingly obtained from the quantum dots at an enhanced emission rate. The underlying radiation mechanism involves the near‐field excitation of surface plasmon polaritons at the metal film, and their selective diffractive scattering by the metasurface into well‐collimated beams along predetermined geometrically tunable directions. These results underscore the distinctive ability of metasurfaces to control radiation properties directly at the source level, which is technologically significant for the continued miniaturization and large‐scale integration of optoelectronic devices.
Substrate-enhanced photothermal nano-imaging of surface polaritons in monolayer graphene
Surface polaritons comprise a wealth of light–matter interactions with deep sub-wavelength scale confinement of electromagnetic modes. However, their nanoscale localized dissipation and thermalization processes are not readily accessible experimentally. Here, we introduce photothermal force microscopy to image surface plasmon polaritons (SPPs) in monolayer graphene through their non-radiative SiO2 substrate dissipation. We demonstrate the real-space SPP imaging via photo-induced atomic force detection, and from comparison with scattering-type scanning near-field optical microscopy imaging attribute the force response to substrate dissipation-enhanced thermal expansion. This work illustrates that nano-optical tip–sample induced dissipative forces facilitate a direct mechanical detection of surface polariton interactions with monolayer sensitivity.
Plasmonics in argentene
Merging concepts from the fields of ab initio materials science and nanophotonics, there is now an opportunity to engineer new photonic materials whose optical, transport, and scattering properties are tailored to attain thermodynamic and quantum limits. Here we present first-principles calculations predicting that Argentene, a single-crystalline hexagonal close-packed monolayer of Ag, can dramatically surpass the optical properties and electrical conductivity of conventional plasmonic materials. In the low-frequency limit, we show that the scattering rate and resistivity reduce by a factor of 3 compared to the bulk three-dimensional metal. Most importantly, the low scattering rate extends to optical frequencies in sharp contrast to, e.g., graphene, whose scattering rate increase drastically in the near-infrared range due to optical-phonon scattering. Combined with an intrinsically high carrier density, this facilitates highly confined surface plasmons extending to visible frequencies. We evaluate Argentene across three distinct figures of merit, in each outperforming the state-of-the-art, making it a valuable addition to the two-dimensional heterostructure toolkit for quantum optoelectronics.
Morphology and property tuning in ZnO–Ni hybrid metamaterials in vertically aligned nanocomposite (VAN) form
ZnO thin films have attracted significant interest in the past decades owing to their unique wide band gap properties, piezoelectric properties, non-linearity and plasmonic properties. Recent efforts have been made in coupling ZnO with secondary phases to enhance its functionalities, such as Au–ZnO nanocomposite thin films with tunable optical and plasmonic properties. In this work, magnetic nanostructures of Ni are incorporated in ZnO thin films in a vertically aligned nanocomposite (VAN) form to couple magnetic and plasmonic response in a complex hybrid metamaterial system. Nickel (Ni) is of interest due to its ferromagnetic and plasmonic properties along with gold (Au) which is also plasmonic. Therefore, two approaches, namely, tuning of the deposition pressure and use of a ZnO–Au seeding layer have been attempted to achieve unique Ni nanostructures in addition to tuning of the microstructure. Together, both approaches demonstrate a range of microstructures such as core–shell, nanodisk, nanocup, and nanocube-like morphologies not previously attempted. Additionally, there is effective tuning of properties. Specifically, the seeding layer thickness causes hyperbolic behavior as well as redshift in the surface plasmon resonance (SPR) wavelength. The addition of the ZnO–Au seeding layer directly influences the optical properties. Plus, regardless of the different approaches, the films demonstrate magnetic anisotropy based on the composition and microstructure of the film which impacted the saturation magnetization and coercivity. This study demonstrates the potential of ZnO-based complex hybrid metamaterials with coupled electro-magneto-optical properties for integrated photonic devices.
Plasmons in the Kagome metal CsV 3 Sb 5
Plasmon polaritons, or plasmons, are coupled oscillations of electrons and electromagnetic fields that can confine the latter into deeply subwavelength scales, enabling novel polaritonic devices. While plasmons have been extensively studied in normal metals or semimetals, they remain largely unexplored in correlated materials. In this paper, we report infrared (IR) nano-imaging of thin flakes of CsV3Sb5, a prototypical layered Kagome metal. We observe propagating plasmon waves in real-space with wavelengths tunable by the flake thickness. From their frequency-momentum dispersion, we infer the out-of-plane dielectric function that is generally difficult to obtain in conventional far-field optics, and elucidate signatures of electronic correlations when compared to density functional theory (DFT). We propose correlation effects might have switched the real part of ϵ c from negative to positive values over a wide range of middle-IR frequencies, transforming the surface plasmons into hyperbolic bulk plasmons, and have dramatically suppressed their dissipation.
ZnO-Au Hybrid Metamaterial Thin Films with Tunable Optical Properties
ZnO-Au nanocomposite thin films have been previously reported as hybrid metamaterials with unique optical properties such as plasmonic resonance properties and hyperbolic behaviors. In this study, Au composition in the ZnO-Au nanocomposites has been effectively tuned by target composition variation and thus resulted in microstructure and optical property tuning. Specifically, all the ZnO-Au nanocomposite thin films grown through the pulsed laser deposition (PLD) method show obvious vertically aligned nanocomposite (VAN) structure with the Au nanopillars embedded in the ZnO matrix. Moreover, the average diameter of Au nanopillars increases as Au concentration increases, which also leads to the redshifts in the surface plasmon resonance (SPR) wavelength and changes in the hyperbolic behaviors of the films. As a whole, this work discusses how strain-driven tuning of optical properties and microstructure resulted through a novel Au concentration variation approach which has not been previously attempted in the ZnO-Au thin film system. These highly ordered films present great promise in the areas of sensing, waveguides, and nanophotonics to name a few.
Formation and optical properties of indium nanoparticle arrays for deep-UV plasmonics
We utilize a combined computational-experimental approach to examine the influence of indium nanoparticle (NP) array distributions on deep-ultraviolet (UV) plasmon resonances. For photon energies < 5.7 eV, analysis of ellipsometric spectra reveals an increase in silicon reflectance induced by indium NP arrays on silicon. For various energies in the range 5.7–7.0 eV, a decrease in reflectance is induced by the NP arrays. Similar trends in reflectance are predicted from finite-difference time-domain (FDTD) simulations using NP size distributions extracted from atomic-force micrographs as input. In addition, in the energy range of 7.4–9.2 eV, the FDTD simulations reveal reflectance minima, characteristic of localized surface plasmon resonances. Here, electron energy-loss spectroscopy collected from individual indium NPs reveals the presence of LSPR at ≈ 8 eV, further supporting the promise of indium NP arrays on silicon for deep-UV plasmonics.
Combined Plasmonic Au-nanoparticle and Conducting Metal Oxide High-temperature Optical Sensing with LSTO
<span style="color: rgba(0, 0, 0, 0.79); font-family: "Source Sans Pro", source-sans-pro, museo_sans300, museo-sans, Arial, sans-serif; font-size: 16px; background-color: rgb(255, 255, 255);">Fiber optic sensor technology offers several advantages for harsh-environment applications. However, the development of optical gas sensing layers that are stable under harsh environmental conditions is an ongoing research challenge. In this work, electronically conducting metal oxide lanthanum-doped strontium titanate (LSTO) films embedded with gold nanoparticles are examined as a sensing layer for application in reducing gas flows at high temperature (600–800 °C). A strong localized surface plasmon resonance (LSPR) based response to hydrogen is demonstrated in the visible region of the spectrum, while a Drude free electron-based response is observed in the near-IR. Characteristics of these responses are studied both on planar glass substrates and on silica fibers. Charge transfer between the oxide film and the gold nanoparticles is explored as a possible mechanism governing the Au LSPR response and is considered in terms of the corresponding properties of the conducting metal oxide-based matrix phase. Principal component analysis is applied to the combined plasmonic and free-carrier based response over a range of temperatures and hydrogen concentrations. It is demonstrated that the combined visible and near-IR response of these films provides improved versatility for multiwavelength interrogation, as well as improved discrimination of important process parameters (concentration and temperature) through application of multivariate analysis techniques.</span>
Precise Colloidal Plasmonic Photocatalysts Constructed by Multistep Photodepositions
Natural photosynthesis relies on a sophisticated charge transfer pathway among multiple components with precise spatial, energetic, and temporal organizations in the aqueous environment. It continues to inspire and challenge the design and fabrication of artificial multicomponent colloidal nanostructures for solar-to-fuel conversion. Herein, we introduce a plasmonic photocatalyst synthesized with colloidal methods with five integrated components including cocatalysts installed in orthogonal locations. The precise deposition of individual inorganic components on an Au/TiO 2 nanodumbell nanostructure is enabled by photoreduction and photo-oxidation, which selectively occurs at the TiO 2 tip sites and Au lateral sites, respectively. Under visible-light irradiation, the photocatalyst exhibited activity of oxygen evolution from water without scavengers. Here, we demonstrate that each component is essential for improving the photocatalytic performance. In addition, mechanistic studies suggest that the photocatalytic reaction requires combining the hot charge carriers derived from exciting both the d-sp interband transition and the localized surface plasmon resonance of Au.
Laterally Modulating Carrier Concentration by Ion Irradiation in CdO Thin Films for Mid‐IR Plasmonics
This report demonstrates tunable carrier densities in CdO thin films through local ion irradiation, providing lateral control of mid‐IR optical properties. Ion‐solid interactions produce donor‐like defects that boost electron concentrations from the practical minimum of 2.5 × 10 19 cm −3 to a maximum of 2.5 × 10 20 cm −3 by metered ion exposure. This range is achieved using He, N, Ar, or Au ions at 1–2.8 MeV; when normalized by displacements per atom, all ion species produce comparable results. Since CdO is well‐described by the Drude model, irradiation‐tuned carrier densities directly alter the infrared dielectric function, and in turn, mid‐infrared optical properties. Further, it is demonstrated that by combining irradiation with traditional lithography, CdO films expose to ions in the presence of 3‐µm thick, patterned photoresist exhibit lateral carrier density profiles with ≈400‐nm resolution. Scanning near‐field optical microscopy reveals sharp optical interfaces with almost no companion contrast in surface morphology, microstructure, or crystallinity. Finally, CdO lateral homostructures supporting surface plasmon polaritons (SPPs) are demonstrated whose dispersion relation can be tuned through periodic patterning in a monolithic platform by simple nanofabrication. Numerical simulations show these polaritons result from strong coupling between excitations at CdO plasma frequencies and SPPs supported by the platinum substrate.
Synchrotron infrared nano-spectroscopy and -imaging
Infrared (IR) spectroscopy has evolved into a powerful analytical technique to probe molecular and lattice vibrations, low-energy electronic excitations and correlations, and related collective surface plasmon, phonon, or other polaritonic resonances. In combination with scanning probe microscopy, near-field infrared nano-spectroscopy and -imaging techniques have recently emerged as a frontier in imaging science, enabling the study of complex heterogeneous materials with simultaneous nanoscale spatial resolution and chemical and quantum state spectroscopic specificity. Here, we describe synchrotron infrared nano-spectroscopy (SINS), which takes advantage of the low-noise, broadband, high spectral irradiance, and coherence of synchrotron infrared radiation for near-field infrared measurements across the mid- to far-infrared with nanometer spatial resolution. This powerful combination provides a qualitatively new form of broadband spatio-spectral analysis of nanoscale, mesoscale, and surface phenomena that were previously difficult to study with IR techniques, or even any form of micro-spectroscopy in general. We review the development of SINS, describe its technical implementations, and highlight selected examples representative of the rapidly growing range of applications in physics, chemistry, biology, materials science, geology, and atmospheric and space sciences.
Comparison of Metal Adhesion Layers for Au Films in Thermoplasmonic Applications
If thermoplasmonic applications such as heat-assisted magnetic recording are to be commercially viable, it is necessary to optimize both thermal stability and plasmonic performance of the devices involved. In this work, a variety of different adhesion layers were investigated for their ability to reduce dewetting of sputtered 50 nm Au films on SiO 2 substrates. Traditional adhesion layer metals Ti and Cr were compared with alternative materials of Al, Ta, and W. Film dewetting was shown to increase when the adhesion material diffuses through the Au layer. An adhesion layer thickness of 0.5 nm resulted in superior thermomechanical stability for all adhesion metals, with an enhancement factor of up to 200X over 5 nm thick analogues. The metals were ranked by their effectiveness in inhibiting dewetting, starting with the most effective, in the order Ta > Ti > W > Cr > AI. Finally, the Au surface-plasmon polariton response was compared for each adhesion layer, and it was found that 0.5 nm adhesion layers produced the best response, with W being the optimal adhesion layer material for plasmonic performance.
Plasmonic Ag nanocomposite phosphate glasses produced via γ-ray irradiation as reduction route
This paper reports on the impact of γ-ray irradiation (10, 100 kGy) on melt-quenched Ag + -doped phosphate glass and the effects of subsequent thermal processing leading to the production of plasmonic Ag nanocomposites. The γ-irradiated glasses were characterized alongside the pristine by differential scanning calorimetry (DSC), Raman spectroscopy, electron paramagnetic resonance (EPR) spectroscopy, optical absorption, and photoluminescence (PL) spectroscopy. DSC characterization showed consistent glass transition temperatures (T g ) before and after γ-irradiation whereas the crystallization temperatures tended to decrease with increasing γ-ray dose. However, a lack of alteration of the glass network structure was supported by Raman spectroscopy. Room temperature EPR spectra clearly showed the formation of phosphorus oxygen hole center (POHC) defects in the undoped host, in addition to another doublet likely associated with a P 3 defect. The presence of paramagnetic silver species encompassing Ag 2+ and 107/109 Ag 0 atoms was also indicated in the silver-activated glass together with POHC defects. Optical absorption spectra were also consistent with the presence of various radiation-induced centers. Further analyzing the glass absorption edge via Tauc plots suggested the formation of electron center (EC) defects in γ-irradiated samples wherein the silver-doped glass exhibited decreasing band gap energies with increasing γ-ray dose. The PL characterization showed the silver-related radio-PL effect was induced exhibiting broad band emission with two maxima around 500 and 625 nm stemming from various molecular Ag$^{x+}_{n}$ clusters. Emission decay analyses revealed that the longer wavelength emission exhibited slower decay. The highest radiation dose of 100 kGy however resulted in weaker emission and faster decay kinetics attributed to energy transfer between the luminescent silver species and POHC defects. Finally subjecting the γ-irradiated Ag-doped glasses to heat treatment near the T g at 490 °C led to the development of the surface plasmon resonance of Ag nanoparticles (NPs) and the vanishing of the Ag$^{x+}_{n}$ clusters luminescence. In conclusion, the presence of the matrix-related EC defects was deemed accountable for the thermally induced reduction and consequent precipitation of Ag NPs making the plasmonic glasses attractive for photonic applications such as nonlinear optics.