High-strength magnetically switchable plasmonic nanorods assembled from a binary nanocrystal mixture
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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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<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>
The tunability of the longitudinal localized surface plasmon resonances (LSPRs) of metallic nanoarcs is demonstrated with key relationships identified between geometric parameters of the arcs and their resonances in the infrared. The wavelength of the LSPRs is tuned by the mid-arc length of the nanoarc. The ratio between the attenuation of the fundamental and second order LSPRs is governed by the nanoarc central angle. Beneficial for plasmonic enhancement of harmonic generation, these two resonances can be tuned independently to obtain octave intervals through the design of a non-uniform arc-width profile. Because the character of the fundamental LSPR mode in nanoarcs combines an electric and a magnetic dipole, plasmonic nanoarcs with tunable resonances can serve as versatile building blocks for chiroptical and nonlinear optical devices.
Cellulose nanocrystals (CNCs) can be attractive templates for the generation of functional inorganic/organic nanoparticles, given their fine sizes, aspect ratios, and sustainable worldwide availability in abundant quantities. Here we present for the first time a scalable, surfactant-free, tailorable wet chemical process for converting commercially-available CNCs into individual aspected gold nanoshell-bearing particles with tunable surface plasmon resonance bands. Using a rational cellulose functionalization approach, stable suspensions of positively-charged CNCs have been generated. Continuous, conductive, nanocrystalline gold coatings were then applied to the individual, electrostatically-stabilized CNCs via decoration with 1-3 nm diameter gold particles followed by electroless gold deposition. Optical analyses indicated that these core-shell nanoparticles exhibited two surface plasmon absorbance bands, with one located in the visible range (near 550 nm) and the other at near infrared wavelengths. Here, the near IR band possessed a peak maximum wavelength that could be tuned over a wide range (1000-1300 nm) by adjusting the gold coating thickness. The bandwidth and wavelength of the peak maximum of the near IR band were also sensitive to the particle size distribution and could be further refined by fractionation using viscosity gradient centrifugation.
This paper reports a robust and stretchable nanolaser platform that can preserve its high mode quality by exploiting hybrid quadrupole plasmons as an optical feedback mechanism. Increasing the size of metal nanoparticles in an array can introduce ultra-sharp lattice plasmon resonances with out-of-plane charge oscillations that are tolerant to lateral strain. By patterning these nanoparticles onto an elastomeric slab surrounded by liquid gain, we realized reversible, tunable nanolasing with high strain sensitivity and no hysteresis. Furthermore, our semi-quantum modeling demonstrates that lasing build-up occurs at the hybrid quadrupole electromagnetic hot spots, which provides a route towards mechanical modulation of light-matter interactions on the nanoscale.
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Nanoparticle-based platforms are gaining strong interest in plant biology and bioenergy research to monitor and control biological processes in whole plants. However, in vivo monitoring of biomolecules using nanoparticles inside plant cells remains challenging due to the impenetrability of the plant cell wall to nanoparticles beyond the exclusion limits (5-20 nm). To overcome this physical barrier, we have designed unique bimetallic silver-coated gold nanorods (AuNR@Ag) capable of entering plant cells, while conserving key plasmonic properties in the near-infrared (NIR). To demonstrate cellular internalization and tracking of the nanorods inside plant tissue, we used a comprehensive multimodal imaging approach that included transmission electron microscopy (TEM), confocal fluorescence microscopy, two-photon luminescence (TPL), X-ray fluorescence microscopy (XRF), and photoacoustics imaging (PAI). We successfully acquired SERS signals of nanorods in vivo inside plant cells of tobacco leaves. On the same leaf samples, we applied orthogonal imaging methods, TPL and PAI techniques for in vivo imaging of the nanorods. This study first demonstrates the intracellular internalization of AuNR@Ag inside whole plant systems for in vivo SERS analysis in tobacco cells. This work demonstrates the potential of this nanoplatform as a new nanotool for intracellular in vivo biosensing for plant biology.
A double-patterning process for scalable, efficient, and deterministic nanoring array fabrication is presented. It enables gaps and features below a size of 20 nm. A writing time of 3 min/cm{sup 2} makes this process extremely appealing for scientific and industrial applications. Numerical simulations are in agreement with experimentally measured optical spectra. Therefore, a platform and a design tool for upcoming next generation plasmonic devices like hybrid plasmonic quantum systems are delivered.
Analyzing the polarization of a circularly polarized light is a critical issue. We have fabricated a spiral nano-structure on the Au film by using focused ion beam etching technique. The fabricated structure can be used as a plasmonic circular polarization analyzer. By designing the relative orientation of two nano-apertures in the spiral structural unit, the propagation direction of the surface plasmon polaritons excited by circularly polarized light of opposite handedness can be controlled. Therefore, the spiral structure could be used to accurately determine the helicity of the excited circularly polarized light. Based on the results of scanning near-field optical microscopy, the obtained circular polarization extinction ratio of this structure was above 500. This structure can be used for a flexible detecting size and a very wide spectrum.
We report the design and experimental realization of a type of miniaturized device for efficient unidirectional launching and shaping of surface plasmon polaritons (SPPs). Each device consists of an array of evenly spaced gap plasmon resonators with varying dimensions. Particle swarm optimization is used to achieve a theoretical two-dimensional launching efficiency of about 51%, under the normal illumination of a 5-μm waist Gaussian beam at 780 nm. By modifying the wavefront of the SPPs, unidirectional SPPs with focused, Bessel, and Airy profiles are launched and imaged with leakage radiation microscopy.
Ultrafast intense photoexcitation of a silicon surface is complementarily studied experimentally and theoretically, with its prompt optical dielectric function obtained by means of time-resolved optical reflection microscopy and the underlying electron-hole plasma dynamics modeled numerically, using a quantum kinetic approach. The corresponding transient surface plasmon-polariton (SPP) dispersion curves of the photo-excited material were simulated as a function of the electron-hole plasma density, using the derived optical dielectric function model, and directly mapped at several laser photon energies, measuring spatial periods of the corresponding SPP-mediated surface relief nanogratings. The unusual spectral dynamics of the surface plasmon resonance, initially increasing with the increase in the electron-hole plasma density but damped at high interband absorption losses induced by the high-density electron-hole plasma through instantaneous bandgap renormalization, was envisioned through the multi-color mapping.
The nanoscale manipulation of matter allows properties to be created in a material that would be difficult or even impossible to achieve in the bulk state. Progress towards such functional nanoscale architectures requires the development of methods to precisely locate nanoscale objects in three dimensions and for the formation of rigorous structure–function relationships across multiple size regimes (beginning from the nanoscale). Here, we use DNA as a programmable ligand to show that two- and three-dimensional mesoscale superlattice crystals with precisely engineered optical properties can be assembled from the bottom up. The superlattices can transition from exhibiting the properties of the constituent plasmonic nanoparticles to adopting the photonic properties defined by the mesoscale crystal (here a rhombic dodecahedron) by controlling the spacing between the gold nanoparticle building blocks. Furthermore, we develop a generally applicable theoretical framework that illustrates how crystal habit can be a design consideration for controlling far-field extinction and light confinement in plasmonic metamaterial superlattices.
Quantum-mechanical effects can result in qualitatively different (and sometimes completely opposite) results for excitation energy transfer in plasmonic waveguides.
Electrochromic polymer infused plasmonic nanohole array shows heterogeneous forward and backward optical scattering response upon polymer electrical permittivity modulation.
Most recent experiments on the excitation of the two plasmon-decay (TPD) instability involve a three-dimensional (3D) array of overlapping laser beams. Our recent two dimensional (2D) simulations suggested that Langmuir cavitation and collapse are important nonlinear saturation mechanisms for TPD. There are important quantitative differences in the Langmuir collapse process in 2D and 3D. To address these and other issues, we have developed a 3D Zakharov code. It has been applied to study the evolution of TPD from absolute instabilities (arising from 3D laser geometries) to the nonlinear state (J. Zhang et al., Phys. Rev. Lett. (submitted)). The present paper concentrates on the nonlinear saturated state excited by the collective action of two crossed laser beams with arbitrary polarizations. Remarkable agreement between 3D and 2D simulations is found for several averaged physical quantities when the beams are polarized in their common plane. As in the previous 2D simulations, we find: (a) the collective, initially convectively unstable triad modes dominate after a sub-picosecond burst, (b) Langmuir cavitation and collapse are important nonlinearities, and (c) that the statistics of intense cavitons are characteristic of a Gaussian random process. The 3D steady-state saturated Langmuir energy level is about 30% higher than in 2D. The auto-correlation functions of the Langmuir envelope field and of the low-frequency electron density field yield the spatial shape of the strongest collapsing cavitons which are 3D ellipsoids whose orientation depends on the laser polarizations. This tilting of the caviton's strongest electric field direction away from the normal to the target surface is a major new 3D result. This tilting may deflect the hot electron flux and thereby mitigate target preheat.
A model for the interaction between the laser light and the plasma waves near the quarter-critical density in plasmas has been studied. This model includes, but is not limited to, the instabilities of two-plasmon decay (TPD) and stimulated Raman scattering (SRS). The full simulation results show the instability growth in the wavevector domains corresponding to TPD and SRS, respectively, and the domain between those two. The instability growth rates and thresholds can be calculated in our model for the parameters of the inertial confinement fusion experiments without the approximations common in analytical theories.
Monolayer transition metal dichalcogenides, coupled to metal plasmonic nanocavities, have recently emerged as new platforms for strong light–matter interactions. These systems are expected to have nonlinear-optical properties that will enable them to be used as entangled photon sources, compact wave-mixing devices, and other elements for classical and quantum photonic technologies. Here, we report the first experimental investigation of the nonlinear properties of these strongly coupled systems, by observing second harmonic generation from a WSe 2 monolayer strongly coupled to a single gold nanorod. In this work, the pump-frequency dependence of the second-harmonic signal displays a pronounced splitting that can be explained by a coupled-oscillator model with second-order nonlinearities. Rigorous numerical simulations utilizing a nonperturbative nonlinear hydrodynamic model of conduction electrons support this interpretation and reproduce experimental results. Our study thus lays the groundwork for understanding the nonlinear properties of strongly coupled nanoscale systems.