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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Charge Transfer Plasmonics in Bespoke Graphene/α-RuCl 3 Cavities

Surface plasmon polaritons (SPPs) provide a window into the nano-optical, electrodynamic response of their host material and its dielectric environment. Graphene/α-RuCl 3 serves as an ideal model system for imaging SPPs since the large work function difference between these two layers facilitates charge transfer that hole dopes graphene with n ~ 10 13 cm –2 free carriers. In this work, we study the emergent THz response of graphene/α-RuCl 3 heterostructures using our home-built cryogenic scanning near-field optical microscope. Using phase-resolved imaging, we clearly observe long wavelength, heavily damped THz SPPs in a series of variable-size graphene cavities. From this, we extract the plasmonic wavelength and scattering rate in the graphene/α-RuCl 3 heterostructures. We determine that the measured plasmon wavelength and electronic scattering rate match our heterostructures’ theoretically predicted values. Here, our results demonstrate that shaping graphene into bespoke cavity structures enables observation and quantification of SPPs in heavily doped graphene that are largely not addressable with other experimental techniques. Moreover, the manifest lack of metallicity observed in the adjacent doped α-RuCl 3 layer provides significant constraints on the nature of the interfacial charge transfer in this 2D heterostructure.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Probing Surface Plasmon Dynamics in Periodic Nanostructures through Ultrafast Electron Microscopy

Surface plasmon polaritons (SPPs) can be manipulated to localize and guide light in subwavelength distances, enabling them to find applications in a wide range of areas, from sensing to quantum computing. Among several methods of SPP excitation, periodic arrays of nano- and microstructures are of particular interest, as they enable engineering SPP properties through structural parameters. Here, in this study, using the photon-induced near-field electron microscopy (PINEM) technique, we investigated the mode formation, coupling, interference, and decay of SPPs in square and hexagonal arrays of circular nanoholes under both visible and near-infrared excitation. Polarization-resolved analysis revealed the key factors governing SPP localization and interference patterns, showing that the periodicity and symmetry of the array primarily determine the SPP interference patterns and their orientation, while pump polarization mainly modulates their intensity. Time-resolved PINEM measurements demonstrated the spatial dependence of the SPP temporal characteristics. In addition, cathodoluminescence (CL) spectroscopy was employed to examine the intrinsic plasmonic characteristics of the structure. Finite difference time domain (FDTD) simulations showed strong agreement with both PINEM and CL measurements on the spatial and spectral behavior of SPPs. Understanding the spatiotemporal dynamics of SPPs on nanostructures beyond the diffraction limit is crucial for optimizing plasmonic structures for advanced photonic and quantum technologies.

Plasmonics↗
DOE OSTI2016

Excitation and propagation of surface plasmon polaritons on a non-structured surface with a permittivity gradient

Accompanied by the rise of plasmonic materials beyond those based on noble metals and the development of advanced materials processing techniques, it is important to understand the plasmonic behavior of materials with large-scale inhomogeneity (such as gradient permittivity materials) because they cannot be modeled simply as scatterers. In this paper, we theoretically analyze the excitation and propagation of surface plasmon polaritons (SPPs) on a planar interface between a homogeneous dielectric and a material with a gradient of negative permittivity. We demonstrate the following: (i) free-space propagating waves and surface waves can be coupled by a gradient negative-permittivity material and (ii) the coupling can be enhanced if the material permittivity variation is suitably designed. This theory is then verified by numerical simulations. A direct application of this theory, ‘rainbow trapping’, is also proposed, considering a realistic design based on doped indium antimonide. This theory may lead to various applications, such as ultracompact spectroscopy and dynamically controllable generation of SPPs.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Plasmon-enhanced ultralow-threshold solid-state triplet fusion upconversion

Triplet fusion upconversion has potential applications in solar cells, photoredox catalysis, additive manufacturing and bioimaging. However, solid-state upconversion systems have struggled to measure up to their solution-phase counterparts, often requiring enormous optical power densities to operate at the maximum efficiency. Here we substantially improve the performance of upconversion films through excitation with surface plasmons that propagate along a planar silver-film interface, leading to an absorption enhancement that reduces the intensity threshold I th by a factor of 19 and enhances the external quantum efficiency by a factor of 17. From this, we achieve I th values as low as 3.4 mW cm −2 and an external quantum efficiency up to 0.094%. To demonstrate real-world viability, we couple the upconversion film to plasmons generated by the near-field of excitons in an organic light-emitting diode. As a result, this scheme is then used to fabricate a white-emitting organic light-emitting diode where blue emission sources from plasmon-excited upconversion, achieving a high colour rendering index of 86.2 and setting precedent for blue emission in the absence of high-energy polarons or triplets.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Bayesian inference for plasmonic nanometrology

Here, we introduce a Bayesian method for the characterization of plasmonic nanoparticles, which is applicable to both near- and far-field problems. Designed to combine data generated from any photon-plasmon interaction experiment with physically motivated theoretical models, our approach leverages state-of-the-art Markov chain Monte Carlo sampling techniques and returns parameter estimates on nanometric scales. Simulated spectral data sets, describing resonant scattering of photons from ellipsoidal and toroidal nanoparticles, are explored as concrete examples of our approach, with the resulting Bayesian estimates showing excellent agreement with the ground truth, even under conditions of high statistical noise. By incorporating Bayes factors into the method as well, we reveal how model selection can determine which one of competing geometric shapes better explains the observed data. Our comprehensive nanometrology procedure can be tailored to a variety of light-particle interaction models, and its reliance on Bayesian inference furnishes automatic uncertainty quantification. In addition to applicability to a host of plasmonic configurations such as nanoparticle dimers, trimers, and array studies, it is proposed that the presented analysis can be extended to the quantum regime, where nonclassical photon statistics may provide additional insight for inference of scatterer properties.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Model for describing plasmonic nanolasers using Maxwell-Liouville equations with finite-difference time-domain calculations

In this work, we present a theoretical study of lasing action when plasmonic metallic structures that show lattice plasmon resonances are embedded in a gain medium. Our model combines classical electrodynamics for arrays of gold nanoparticles with a four-level quantum Liouville model of the laser dye photophysics. A numerical solution was implemented using finite-difference time-domain calculations coupled with a finite-difference solution to the Liouville equation. A particular focus of this work is the influence of dephasing in the quantum dynamics on the emission intensity at the threshold for lasing. We find that dephasing in the quantum system leads to reduced lasing emission, but with little effect on the long-term population inversion. Both electronic and vibrational dephasing is considered, but only electronic dephasing is significant, with the fully dephased result appearing for dephasing times comparable to plasmon dephasing (~10 fs) while fully coherent results involve >100 ps dephasing times as determined by the rate of stimulated emission. There are factor-of-2 differences between the Maxwell-Liouville results (greater emission intensities and narrower widths) compared to the corresponding results of rate-equation models of the dye states, which indicates the importance of using the Maxwell-Liouville approach in modeling these systems. We also examine rate-equation models with and without constraints arising from the Pauli exclusion principle, and we find relatively small effects.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Spatiotemporal imaging of plasmonic fields near nanoparticles below the diffraction limit

Optically induced collective conduction-electron oscillations can generate intense plasmonic fields near metallic nanoparticles. Here, we suggest a method for reconstructing such nanoplasmonic fields with nanometer spatial and sub-femtosecond temporal resolution from streaked photoemission spectra. Applying this imaging scheme to Au nanospheres, we demonstrate the accurate spatiotemporal reconstruction of the plasmonic near-field distribution in comparison with the directly calculated plasmonic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Two-Photon Spontaneous Emission in Atomically Thin Plasmonic Nanostructures

The ability to harness light-matter interactions at the few-photon level plays a pivotal role in quantum technologies. Single photons—the most elementary states of light—can be generated on demand in atomic and solid state emitters. Two-photon states are also key quantum assets, but achieving them in individual emitters is challenging because their generation rate is much slower than competing one-photon processes. We demonstrate that atomically thin plasmonic nanostructures can harness two-photon spontaneous emission, resulting in giant far field two-photon production, a wealth of resonant modes enabling tailored photonic and plasmonic entangled states, and plasmon-assisted single-photon creation orders of magnitude more efficient than standard one-photon emission. We unravel the two-photon spontaneous emission channels and show that their spectral line shapes emerge from an intricate interplay between Fano and Lorentzian resonances. Enhanced two-photon spontaneous emission in two-dimensional nanostructures paves the way to an alternative efficient source of light-matter entanglement for on-chip quantum information processing and free-space quantum communications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Toward white light emission from plasmonic-luminescent hybrid nanostructures

We study the light emission of plasmonic-luminescent hybrid nanostructures consisting of Ag nanoparticles (NPs) embedded in europium oxide (EuO X ). The Ag NPs present a bidimensional organization in the nanostructures and they optically behave as oblate spheroids. The photoluminescence (PL) spectral response of the nanostructures evolves from a narrow red emission characteristic of Eu 3+ ions in absence of Ag NPs to a broad blue-green emission band associated with Eu 2+ ions when the layer of Ag NPs is present. This behavior is not related to a change in the Eu 2+ /Eu 3+ ratio, which is verified by compositional analysis. Instead, a detailed investigation of the PL emission of the nanostructures suggests that the coupling of the Ag NPs to the Eu 2+ ions present in the EuO X layer, which manifests itself in an efficient sensitization of these ions, enhances their broad visible emission. In particular, the longitudinal mode of the Ag NPs surface plasmon is considered to be responsible for the efficient energy transfer for the non-normal incidence excitation PL configuration used. Finally, the use of a capping amorphous Al 2 O 3 layer allows improving the robustness of hybrid nanostructures and further enhances their PL emission. These findings provide a new path to actively control the selective excitation of Eu 2+ and Eu 3+ ions via a controlled coupling with the surface plasmon resonance modes of the Ag NPs and points to these nanostructures as promising building blocks for the development of integrable white light sources.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Plasmon Mediated Near–Field Energy Transfer From Solid–State, Electrically Injected Excitons to Solution Phase Chromophores

An organic diode is demonstrated that near-field energy transfers to molecules in solution via surface plasmon polaritons, in contrast to typical far-field excitation via absorption of traveling photons. Electrically generated excitons couple to surface plasmon modes in the cathode; the plasmons subsequently excite chromophore molecules on top of the cathode. External quantum efficiency and time resolved photoluminescence measurements are used to characterize the diode and the near-field energy transfer process. In addition, it is shown that excited chromophores can charge-transfer to quencher molecules, illustrating the potential of this device to be used for photochemical applications.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2024

Engineering Ultrathin Alloy Shell in Au@AuPd Core-Shell Nanoparticles for Efficient Plasmon-Driven Photocatalysis

Bimetallic core-shell nanoparticles (NPs) possessing a synergetic coupling of plasmonic and catalytic metals have emerged as promising prototypes for efficient plasmon-driven photocatalysis. Here, Au@AuPd core-shell NPs composed of Au core NP and ultrathin AuPd shell are introduced to acquire improved light utilization efficiency in photocatalytic selective oxidation. With systematical control of the composition of the ultrathin alloy shell, it reveals that the Au@AuPd core-shell NPs with 10 at% Pd (in the single-atom alloy regime) is an effective nanostructure capable of maximizing the quantum yield of plasmon-induced light absorption and optimizing the surface electronic structure for catalytic reactions. This controlled system provides new insights into shell engineering for enhancing photocatalytic performance via the regulation of energy funneling processes in core-shell nanocatalysts.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Graphene Plasmonics: A Platform for 2D Optics

2D optics is gradually emerging as a frontier in modern optics. Plasmons in graphene provide a prominent platform for 2D optics in which the light is squeezed into atomic scale. This report highlights some recent progresses in graphene plasmons toward the 2D optics. The launch, observation, and advanced manipulation of propagating graphene plasmons for 2D optical circuits are described. Representative achievements associated with graphene metasurfaces, challenges, recent progresses like photoexcited graphene metasurfaces, and the transformation optics linking 2D to bulk optics with singularity are investigated.

2D optics↗
DOE OSTI2018

Self-Assembled Ag–TiN Hybrid Plasmonic Metamaterial: Tailorable Tilted Nanopillar and Optical Properties

Key challenges limiting the adoption of metallic plasmonic nanostructures for practical devices include structural stability and the ease of large-scale fabrication. Overcoming these issues may require novel metamaterial fabrication with potentials for improved durability under extreme conditions. Here, in this paper, a self-assembled growth of a hybrid plasmonic metamaterial in thin-film form is reported, with epitaxial Ag nanopillars embedded in TiN, a mechanically strong and chemically inert matrix. One of the key achievements lies in the successful control of the tilt angle of the Ag nanopillars (from 0° to 50°), which is attributed to the interplay between the growth kinetics and thermodynamics during deposition. Such an anisotropic nature offered by the tilted Ag nanopillars in TiN matrix is crucial for achieving broadband, asymmetric optical selectivity. Optical spectra coupled with numerical simulations demonstrate strong plasmonic resonance, as well as angular selectivity in a broad UV–vis to near-infrared regime. The nanostructured metamaterials in this work, which consist of highly conductive metallic nanopillars in a durable nitride matrix, have the potential to serve as a novel hybrid material platform for highly tailorable nanoscale metamaterial designs, suitable for high temperature optical applications.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Separating Physically Distinct Mechanisms in Complex Infrared Plasmonic Nanostructures via Machine Learning Enhanced Electron Energy Loss Spectroscopy

Electron energy loss spectroscopy (EELS) enables direct exploration of plasmonic phenomena at the nanometer level. To isolate individual plasmon modes, linear unmixing methods can be used to separate different physical mechanisms, but in larger and more complex systems the interpretability of the components becomes uncertain. Here, infrared plasmonic resonances in self-assembled heterogeneous monolayer films of doped-semiconductor nanoparticles are examined beyond linear unmixing techniques, and both supervised and unsupervised machine-learning-based analyses of hyperspectral EELS datasets are demonstrated. Additionally, in the supervised approach, a human operator labels a small number of pixels in the hyperspectral dataset corresponding to features of interest which are then propagated across the entire dataset. In the unsupervised approach, non-linear autoencoders are used to create a highly-reduced latent-space representation of the dataset, within which insight into the relevant physics can be gleaned from straightforward distance metrics that do not depend on operator input and bias. The advantage of these approaches is that the labeling separates physical mechanisms without altering the data, enabling robust analyses of the influence of heterogeneities in mesoscale complex systems.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Nematic Order, Plasmonic Switching and Self-Patterning of Colloidal Gold Bipyramids

Dispersing inorganic colloidal nanoparticles within nematic liquid crystals provides a versatile platform both for forming new soft matter phases and for predefining physical behavior through mesoscale molecular-colloidal self-organization. However, owing to formation of particle-induced singular defects and complex elasticity-mediated interactions, this approach has been implemented mainly just for colloidal nanorods and nanoplatelets, limiting its potential technological utility. Here, orientationally ordered nematic colloidal dispersions are reported of pentagonal gold bipyramids that exhibit narrow but controlled polarization-dependent surface plasmon resonance spectra and facile electric switching. Bipyramids tend to orient with their C 5 rotation symmetry axes along the nematic director, exhibiting spatially homogeneous density within aligned samples. Topological solitons, like heliknotons, allow for spatial reorganization of these nanoparticles according to elastic free energy density within their micrometer-scale structures. With the nanoparticle orientations slaved to the nematic director and being switched by low voltages ≈1 V within a fraction of a second, these plasmonic composite materials are of interest for technological uses like color filters and plasmonic polarizers, as well as may lead to the development of unusual nematic phases, like pentatic liquid crystals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Predictability of Localized Plasmonic Responses in Nanoparticle Assemblies

Design of nanoscale structures with desired optical properties is a key task for nanophotonics. In this work, the correlative relationship between local nanoparticle geometries and their plasmonic responses is established using encoder-decoder neural networks. In the im2spec network, the relationship between local particle geometries and local spectra is established via encoding the observed geometries to a small number of latent variables and subsequently decoding into plasmonic spectra; in the spec2im network, the relationship is reversed. Surprisingly, these reduced descriptions allow high-veracity predictions of local responses based on geometries for fixed compositions and surface chemical states. Analysis of the latent space distributions and the corresponding decoded and closest (in latent space) encoded images yields insight into the generative mechanisms of plasmonic interactions in the nanoparticle arrays. Ultimately, this approach creates a path toward determining configurations that yield the spectrum closest to the desired one, paving the way for stochastic design of nanoplasmonic structures.

nanoparticle arrays↗
DOE OSTI2018

Plasmon-Polaritons in Island Metal Films: A Solution in the Framework of the Coherent Potential Approximation

The photon propagator describing the interaction of light with a monolayer of metal particles (island film) is calculated in the coherent potential approximation. It is shown that the shift in the frequency peak of a dipole surface plasmon for a monolayer particle relative to the analogous frequency of the plasma resonance for an isolated particle is not the only manifestation of the influence of neighboring particles. Neighboring particles also produce a bimodal structure in the spectrum line of the plasmon resonance. The possibility of fine structure in the plasmon resonance spectrum lines is predicted.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Design considerations of highly efficient D-shaped plasmonic biosensor

Design considerations of photonic crystal fiber (PCF) surface plasmon biosensor with high sensitivity to monitor glucose concentration is reported and studied. Based on a well-known large mode area (LMA) single mode PCF, two different configurations have been studied to investigate the impact of the etching process on the biosensor sensitivity. Furthermore, the possibility of infiltrating one hole by a plasmonic material to increases the biosensor sensitivity is studied. A full vectorial finite element method (FVFEM) is used to carry out the analysis of the reported biosensor. In addition, the geometrical parameters of the suggested biosensors have been optimized to obtain the highest sensitivity. The suggested biosensor based on a D-shaped PCF with plasmonic rod achieves sensitivity as high as 13,600 nm/RIU with corresponding resolution of 7.35×10{sup −6} RIU.The analysis also reveals that the proposed biosensor has a linear performance which is needed practically. Therefore, the reported biosensor has advantages in terms of fabrication feasibility and high linear sensitivity.

36 MATERIALS SCIENCE↗