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Results for “nanoplasmonic”

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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13 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Physics Discovery in Nanoplasmonic Systems via Autonomous Experiments in Scanning Transmission Electron Microscopy

Abstract Physics‐driven discovery in an autonomous experiment has emerged as a dream application of machine learning in physical sciences. Here, this work develops and experimentally implements a deep kernel learning (DKL) workflow combining the correlative prediction of the target functional response and its uncertainty from the structure, and physics‐based selection of acquisition function, which autonomously guides the navigation of the image space. Compared to classical Bayesian optimization (BO) methods, this approach allows to capture the complex spatial features present in the images of realistic materials, and dynamically learn structure–property relationships. In combination with the flexible scalarizer function that allows to ascribe the degree of physical interest to predicted spectra, this enables physical discovery in automated experiment. Here, this approach is illustrated for nanoplasmonic studies of nanoparticles and experimentally implemented in a truly autonomous fashion for bulk‐ and edge plasmon discovery in MnPS 3 , a lesser‐known beam‐sensitive layered 2D material. This approach is universal, can be directly used as‐is with any specimen, and is expected to be applicable to any probe‐based microscopic techniques including other STEM modalities, scanning probe microscopies, chemical, and optical imaging.

42 ENGINEERING↗
DOE OSTI2021

Develop On-Demand nanoplasmonic Device Concepts in a Semiconductor Compatible Hybrid System. Final Report

This report summarizes the research activities supported by the U.S. Department of Energy grant DE-SC-0010399. The goal of this project is to is to develop an on-demand nanoplasmonic platform that combines emerging oxide nanoelectronics with a low-loss semiconductor-friendly plasmonic materials. Toward this goal, several unique heterostructures formed between complex oxides and 2D layered materials have been developed. Based on these material systems, a set of atomic force microscope (AFM) based techniques have been developed that can allow long-living and reversible material phase transitions to be manipulated in nanoscale at room temperature. Using such technique and through interface coupling, we can effectively tune the plasmon propagations in unconventional plasmonic materials such as graphene and VO 2 . In addition, we also discovered a plethora of novel interface enabled electro-optic effects, including the spatial modulation of light using 2DEG, a giant programmable photothermoelectric effects at room temperature, a light induced superconducting transition, and a tunable giant third order optical nonlinearities. These major results are outlined in this report, along with lists of project participants and products.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Exceptional Points in Novel Multiscale Quantum-Nanoplasmonic Materials for Enhanced Sensing and Other Applications

Lossy quantum systems can display fascinating behaviors around singularities known as exceptional points in their complex eigenvalue spaces. Interest in these systems was ignited over two decades ago when Carl Bender and Stefan Boettcher—a LANL Director’s Postdoctoral Fellow at the time—pointed out that many features of conventional lossless quantum systems, such as real operator eigenvalues, could be recovered in lossy systems exhibiting parity- and time-reversal (ΡΤ) symmetry.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Correlation-driven attosecond photoemission delay in the plasmonic excitation of C60 fullerene

Extreme light confinement in plasmonic nanosystems enables novel applications in photonics, sensor technology, energy harvesting, biology, and quantum information processing. Fullerenes represent an extreme case for nanoplasmonics: they are sub-nanometer carbon- based molecules showing high-energy and ultrabroad plasmon resonances, however the fundamental mechanisms driving the plasmonic response and the corresponding collective electron dynamics are still elusive. Here, we uncover the dominant role of electron correlations in the dynamics of the giant plasmon resonance (GPR) of the sub-nanometer system C60 by employing attosecond photoemission chronoscopy. We find a characteristic photoemission delay of up to about 300 attoseconds that is purely induced by coherent large-scale electron correlations in the plasmonic potential. These results provide novel insights into the nature of the plasmon resonances in sub-nanometer systems and open new perspectives for advancing nanoplasmonic applications.

Biswas, Shubhadeep [SLAC National Accelerator Labo↗
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 OSTI2021

Sculpting the Plasmonic Responses of Nanoparticles by Directed Electron Beam Irradiation

Spatial confinement of matter in functional nanostructures has propelled these systems to the forefront of nanoscience, both as a playground for exotic physics and quantum phenomena and in multiple applications including plasmonics, optoelectronics, and sensing. In parallel, the emergence of monochromated electron energy loss spectroscopy (EELS) has enabled exploration of local nanoplasmonic functionalities within single nanoparticles and the collective response of nanoparticle assemblies, providing deep insight into associated mechanisms. However, modern synthesis processes for plasmonic nanostructures are often limited in the types of accessible geometry, and materials and are limited to spatial precisions on the order of tens of nm, precluding the direct exploration of critical aspects of the structure-property relationships. Here, the atomic-sized probe of the scanning transmission electron microscope is used to perform precise sculpting and design nanoparticle configurations. Using low-loss EELS, dynamic analyses of the evolution of the plasmonic response are provided. It is shown that within self-assembled systems of nanoparticles, individual nanoparticles can be selectively removed, reshaped, or patterned with nanometer-level resolution, effectively modifying the plasmonic response in both space and energy. This process significantly increases the scope for design possibilities and presents opportunities for unique structure development, which are ultimately the key for nanophotonic design.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Building Atomic and Plasmonic Devices via Electron Beams: from Desired Structures to Desired Properties

The evolution of the aberration correction in Scanning Transmission Electron Microscopy (STEM) has enabled multiple advances including high-resolution structural imaging, pm-level position detection of atomic columns, and ~3-5 mV resolution electron energy loss spectroscopy of the chemical and physical functionalities. These developments have further enabled the precise manipulation of the atomic structure of materials, including removal and formation of atomic planes in 3D materials, controlled atomic motion, and even direct atomic assembly of homo- and heteroatomic artificial molecules. Here, we will discuss several recent advances in STEM-EELS automated experiments as applied to quantum and nanoplasmonic systems.

42 ENGINEERING↗
DOE OSTI2020

Plasmon–emitter interactions at the nanoscale

Plasmon–emitter interactions are of central importance in modern nanoplasmonics and are generally maximal at short emitter–surface separations. However, when the separation falls below 10–20 nm, the classical theory deteriorates progressively due to its neglect of quantum effects such as nonlocality, electronic spill-out, and Landau damping. Here we show how this neglect can be remedied in a unified theoretical treatment of mesoscopic electrodynamics incorporating Feibelman d -parameters. Our approach incorporates nonclassical resonance shifts and surface-enabled Landau damping—a nonlocal damping effect—which have a dramatic impact on the amplitude and spectral distribution of plasmon–emitter interactions. We consider a broad array of plasmon–emitter interactions ranging from dipolar and multipolar spontaneous emission enhancement, to plasmon-assisted energy transfer and enhancement of two-photon transitions. The formalism gives a complete account of both plasmons and plasmon–emitter interactions at the nanoscale, constituting a simple yet rigorous platform to include nonclassical effects in plasmon-enabled nanophotonic phenomena.

Science & Technology - Other Topics↗
DOE OSTI2021

Strong Purcell enhancement at telecom wavelengths afforded by spinel Fe 3 O 4 nanocrystals with size-tunable plasmonic properties

Developments in the field of nanoplasmonics have the potential to advance applications from information processing and telecommunications to light-based sensing. Traditionally, nanoscale noble metals such as gold and silver have been used to achieve the targeted enhancements in light-matter interactions that result from the presence of localized surface plasmons (LSPs). However, interest has recently shifted to intrinsically doped semiconductor nanocrystals (NCs) for their ability to display LSP resonances (LSPRs) over a much broader spectral range, including the infrared (IR). Among semiconducting plasmonic NCs, spinel metal oxides (sp-MOs) are an emerging class of materials with distinct advantages in accessing the telecommunications bands in the IR and affording useful environmental stability. In this work, we report the plasmonic properties of Fe 3 O 4 sp-MO NCs, known previously only for their magnetic functionality, and demonstrate their ability to modify the light-emission properties of telecom-emitting quantum dots (QDs). We establish the synthetic conditions for tuning sp-MO NC size, composition and doping characteristics, resulting in unprecedented tunability of electronic behavior and plasmonic response over 450 nm. In particular, with diameter-dependent variations in free-electron concentration across the Fe 3 O 4 NC series, we introduce a strong NC size dependency onto the optical response. In addition, our observation of plasmonics-enhanced decay rates from telecom-emitting QDs reveals Purcell enhancement factors for simple plasmonic-spacer-emitter sandwich structures up to 51-fold, which are comparable to values achieved previously only for emitters in the visible range coupled with conventional noble metal NCs.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Interplay between disorder and collective coherent response: Superradiance and spectral motional narrowing in the time domain

The interplay between static and dynamic disorder and collective optical response in molecular ensembles is an important characteristic of nanoplasmonic and nanophotonic molecular systems. Here we investigate the cooperative superradiant response of a molecular ensemble of quantum emitters under the influence of environmental disorder, including inhomogeneous broadening (as induced by a static random distribution of the molecular transition frequencies) and motional narrowing (as induced by stochastic modulation of these excitation energies). The effect of inhomogeneous broadening is to destroy the coherence of the collective molecular excitation and suppress superradiant emission. However, fast stochastic modulation of the molecular excitation energy can effectively restore the coherence of the quantum emitters and lead to a recovery of superradiant emission, which is an unexpected manifestation of motional narrowing. For a light-scattering process as induced by an off-resonant incident pulse, stochastic modulation leads to inelastic fluorescence emission at the average excitation energy at long times and suggests that dynamic disorder effects can actually lead to collective excitation of the molecular ensemble.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Smartphone-Based Device for Colorimetric Detection of MicroRNA Biomarkers Using Nanoparticle-Based Assay

The detection of microRNAs (miRNAs) is emerging as a clinically important tool for the non-invasive detection of a wide variety of diseases ranging from cancers and cardiovascular illnesses to infectious diseases. Over the years, miRNA detection schemes have become accessible to clinicians, but they still require sophisticated and bulky laboratory equipment and trained personnel to operate. The exceptional computing ability and ease of use of modern smartphones coupled with fieldable optical detection technologies can provide a useful and portable alternative to these laboratory systems. Herein, we present the development of a smartphone-based device called Krometriks, which is capable of simple and rapid colorimetric detection of microRNA (miRNAs) using a nanoparticle-based assay. The device consists of a smartphone, a 3D printed accessory, and a custom-built dedicated mobile app. We illustrate the utility of Krometriks for the detection of an important miRNA disease biomarker, miR-21, using a nanoplasmonics-based assay developed by our group. We show that Krometriks can detect miRNA down to nanomolar concentrations with detection results comparable to a laboratory-based benchtop spectrophotometer. With slight changes to the accessory design, Krometriks can be made compatible with different types of smartphone models and specifications. Thus, the Krometriks device offers a practical colorimetric platform that has the potential to provide accessible and affordable miRNA diagnostics for point-of-care and field applications in low-resource settings.

Krishnan, Tushar (ORCID:0000000342610336)↗
DOE OSTI2022

Strong-Field Control of Plasmonic Properties in Core–Shell Nanoparticles

Utilization of the plasmonic response in nanosystems is a key component of nanophotonics that is typically altered by varying the incident optical frequency or the material configuration. However, in this work we demonstrate that employing intense, femtosecond laser fields unlock nonlinear light–matter interactions such that precise control of the optical response is achieved solely by adjusting the incident intensity. The plasmonic properties of Au/SiO 2 nanoshells are manipulated by exploiting the nonlinear index of refraction of gold and experimentally observed by employing photoelectrons emitted during the interaction as a sensitive, sub-wavelength probe. A striking transition seen in the photoelectron energy spectrum between the weak and strong-field regime is verified by a modified Mie theory simulation that incorporates the nonlinear dielectric nanoshell response. The exhibited intensity-dependent optical control of the plasmonic response in prototypical core–shell nanoparticles paves the way toward ultrafast switching and opto-electronic signal modulation with more complex nanostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗