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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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At least 901 records · Page 50
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Numerical Simulation of Light to Heat Conversion by Plasmonic Nanoheaters

Plasmonic nanoparticles are widely recognized as photothermal conversion agents, i.e., nanotransducers or nanoheaters. Translation of these materials into practical applications requires quantitative analyses of their photothermal conversion efficiencies (η). However, the value of η obtained for different materials is dramatically influenced by the experimental setup and method of calculation. Here, we evaluate the most common methods for estimating η (Roper’s and Wang’s) and compare these with numerical estimates using the simulation software ANSYS. Experiments were performed with colloidal gold nanorod solutions suspended in a hanging droplet irradiated by an 808 nm diode laser and monitored by a thermal camera. The ANSYS simulations accounted for both heating and evaporation, providing η values consistent with the Wang method but higher than the Roper approach. This study details methods for estimating the photothermal efficiency and finds ANSYS to be a robust tool where experimental constraints complicate traditional methods.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Ultrafast Imaging of Surface Plasmons Propagating on a Gold Surface

We record time-resolved nonlinear photoemission electron microscopy (tr-PEEM) images of propagating surface plasmons (PSPs) launched from a lithographically patterned rectangular trench on a flat gold surface. Our tr-PEEM scheme involves a pair of identical, spatially separated, and interferometrically-locked femtosecond laser pulses. Power dependent PEEM images provide experimental evidence for a sequential coherent nonlinear photoemission process, in which one laser source creates a PSP polarization state through a linear interaction, and the second subsequently probes the prepared state via two photon photoemission. The recorded time-resolved movies of a PSP allow us to directly measure various properties of the surface-bound wave packet, including its carrier wavelength (785 nm) and group velocity (0.95c). In addition, tr-PEEM in concert with finite-difference time domain simulations together allow us to set a lower limit of 75 μm for the decay length of the PSP on a 100 nm thick gold film.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2019

Hierarchical Assembly of Plasmonic Nanoparticle Heterodimer Arrays with Tunable Sub-5 nm Nanogaps

Nanoparticle assemblies have generated intense interest because of their novel optical, electronic, and magnetic properties that open up numerous opportunities in fundamental and applied nanophotonics, -electronics, and -magnetics. However, despite the great scientific and technological potential of these structures, it remains an outstanding challenge to reliably fabricate such assemblies with both nanometer-level structural control and precise spatial arrangements on a macroscopic scale. It is the combination of these two features that is key to realizing nanoparticle assemblies potential, particular for device applications. To address this challenge, we propose a hierarchical assembly approach consisting of both template-particle and particle-particle interactions, whereby the former ensures precise addressability of assemblies on a surface and the latter provides nanometer-level structural control. Template-particle interactions are harnessed via chemical-pattern-directed assembly, and the particle-particle interactions are controlled using DNA-directed self-assembly. To demonstrate the potential of this hierarchical assembly approach, we demonstrate the fabrication of a particularly fascinating assembly: the nanoparticle heterodimer, which possesses a surprisingly rich set of plasmonic properties and is a promising candidate to enable a variety of imaging and sensing applications. Each heterodimer is placed on the surface at predetermined locations, and the precise control of the nanogaps is confirmed by far-field scattering measurements of individual dimers. We further demonstrate that the gap size can be effectively tuned by varying the DNA length. By correlating measured spectra with finite-difference time-domain (FDTD) simulations, we determine the gap sizes to be 4.2 and 5.0 nm-with subnm deviation-for the two DNA lengths investigated. This is one of the best gap uniformities ever demonstrated for surface-bound nanoparticle assemblies. The estimated surface-enhanced Raman scattering (SERS) enhancement factor of these heterodimers is on the order of 10 5 -10 6 with high reproducibility and predictable polarization-dependence. This hierarchical fabrication technique-employing both template-particle and particle-particle interactions-constitutes a novel platform for the realization of functional nanoparticle assemblies on surfaces and thereby creates new opportunities to implement these structures in a variety of applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Localized Orbital Excitation Drives Bond Formation in Plasmonic Catalysis

Localized surface plasmons generated on metallic nanostructures can be used to accelerate molecular transformations; however, the efficiency is limited by the challenge to control the energy/charge transfer at the interfaces. Here, we combine density functional theory (DFT) calculations and experiments to reveal the mechanism of nitrophenol reduction on Au nanoparticles under visible-light irradiation and propose a strategy to further enhance the reaction rates. DFT calculations show a reduced activation barrier under electronic excitation on Au(111), thus explaining the measured higher rates under visible-light irradiation. Furthermore, we propose a heterostructure with Au nanoparticles covered by a thin film of hexagonal boron nitride; the latter is used to decouple the molecular orbitals from the metal to enable charge localization in the molecule. DFT calculations show that, by this electronic decoupling, the activation barrier can be lowered by a factor of five. Furthermore, this work thus provides a valuable strategy for optimizing catalytic efficiency.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Plasmonic Conducting Metal Oxide-Based Optical Fiber Sensors for Chemical and Intermediate Temperature-Sensing Applications

The demand for real-time sensors in harsh environments at elevated temperature is significant and increasing. In this manuscript, the chemical and temperature sensing using the optical response through the practical fiber platform is demonstrated, and principle component analysis is coupled with targeted experimental film characterization to understand the fundamental sensing layer properties, which dominate measured gas sensing responses in complex gas mixtures. More specifically, tin-doped indium oxide-decorated sensors fabricated with the sol–gel method show stable and stepwise transmission responses varying over a wide range of H2 concentration (5–100%) at 250–350 °C as well as responses to CH4 and CO to a lesser extent. Measured responses are attributed to modifications to the surface plasmon resonance absorption in the near-infrared range and are dominated by the highest concentrations of the most-reducing analyte based upon systematic mixed gas stream experiments. Principal component analysis is utilized for this type of sensor to improve the quantitative and qualitative understanding of responses, clearly identifying that the dominant principle component (PC #1) accounts for ~78% of total data variance. Correlations between PC #1 and the experimentally derived free carrier concentration confirm that this material property plays the strongest role on the ITO gas sensing mechanism, while correlations between the free carrier mobility and the second most important principle component (PC #2) suggest that this quantity may play a significant but secondary role. As such, the results presented here clarify the relationship between generalized principle components and fundamental sensing materials properties thereby suggesting the pathway toward improved multicomponent gas speciation through sensor layer engineering. Furthermore, the work presented represents a significant step toward the ultimate objective of optical waveguide sensors integrated with multivariate data analytics for multiparameter monitoring with a single sensor element.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Lamellar and Hexagonal Assemblies of PEG-Grafted Silver Nanoparticles: Implications for Plasmonics and Photonics

Assembly of silver nanoparticles (AgNPs) grafted with thiolated poly(ethylene glycol) (PEG-SH) with various molecular weights is reported. Synchrotron-based X-ray surface-sensitive diffraction methods are used to determine the nature of two-dimensional (2D) assemblies at liquid/vapor interfaces, and small-angle X-ray scattering (SAXS) is used to monitor the three-dimensional (3D) assemblies in bulk suspensions. We find that assembly can be induced either by the addition of K 2 CO 3 or polyacrylic acid (PAA) to the PEG-AgNP aqueous suspensions. The addition of K 2 CO 3 induces a 2D hexagonal structure at the liquid/vapor interface and a 3D hexagonal columnar structure in solutions, where the columns consist of tethered PEG-AgNP chains. On the other hand, the addition of PAA leads to the formation of a 2D lamella-like distorted hexagonal sheet at the liquid/vapor interface and a 3D lamellar superstructure formed by stacked 2D sheets in the PEG-AgNP suspension. Effects of the core type of nanoparticles on the assembly can be used to control structures for potential applications in plasmonics and photonics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Active Radiative Thermal Switching with Graphene Plasmon Resonators

We theoretically demonstrate a near-field radiative thermal switch based on thermally excited surface plasmons in graphene resonators. The high tunability of graphene enables substantial modulation of near-field radiative heat transfer, which, when combined with the use of resonant structures, overcomes the intrinsically broadband nature of thermal radiation. In canonical geometries, we use nonlinear optimization to show that stacked graphene sheets offer improved heat conductance contrast between “ON” and “OFF” switching states and that a >10× higher modulation is achieved between isolated graphene resonators than for parallel graphene sheets. In all cases, we find that carrier mobility is a crucial parameter for the performance of a radiative thermal switch. Furthermore, we derive shape-agnostic analytical approximations for the resonant heat transfer that provide general scaling laws and allow for direct comparison between different resonator geometries dominated by a single mode. The presented scheme is relevant for active thermal management and energy harvesting as well as probing excited-state dynamics at the nanoscale.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2016

Size-Dependent Coherent-Phonon Plasmon Modulation and Deformation Characterization in Gold Bipyramids and Nanojavelins

Localized surface plasmon resonances (LSPRs) arising from metallic nanoparticles offer an array of prospective applications that range from chemical sensing to biotherapies. Bipyramidal particles exhibit particularly narrow ensemble LSPR resonances that reflect small dispersity of size and shape but until recently were only synthetically accessible over a limited range of sizes with corresponding aspect ratios. Narrow size dispersion offers the opportunity to examine ensemble dynamical phenomena such as coherent phonons that induce periodic oscillations of the LSPR energy. Here, we characterize transient optical behavior of a large range of gold bipyramid sizes, as well as higher aspect ratio nanojavelin ensembles with specific attention to the lowest-order acoustic phonon mode of these nanoparticles. We report coherent phonon-driven oscillations of the LSPR position for particles with resonances spanning 670 to 1330 nm. Nanojavelins were shown to behave similarly to bipyramids but offer the prospect of separate control over LSPR energy and coherent phonon oscillation period. We develop a new methodology for quantitatively measuring mechanical expansion caused by photogenerated coherent phonons. Using this method, we find an elongation of approximately 1% per photon absorbed per unit cell and that particle expansion along the lowest frequency acoustic phonon mode is linearly proportional to excitation fluence for the fluence range studied. These characterizations provide insight regarding means to manipulate phonon period and transient mechanical deformation.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Plasmonic Hot Hole Transfer in Gold Nanoparticle-Decorated Transition Metal Dichalcogenide Nanosheets

This work studies photogenerated carrier dynamics in gold nanoparticle (AuNP)-decorated mono- to few-layer transition metal dichalcogenide (TMD) nanosheets using transient absorption spectroscopy (TA). TA unveiled the presence of a long-lived photoinduced absorption (PIA) feature in both MoSe 2 and WSe 2 decorated with covalently bound AuNPs. This long-lived PIA feature emerges only from direct Au interband excitation in AuNP-decorated MoSe 2 and WSe 2 ; it does not manifest from intraband excitation nor in AuNP-decorated MoS 2 or WS 2 . Based on X-ray/ultraviolet photoelectron spectroscopy and previous theoretical studies, it is proposed that this PIA signature arises from hot hole transfer from the AuNP to the adjacent TMD, producing a charge-separated state. This suggests charge separation at the metal-semiconductor interface may be used to extend the lifetime of interband excitation generated hot holes. We conclude this development could represent an important advance in harnessing plasmonic dissipation pathways to generate long-lived carriers suited for solar-driven light harvesting and catalysis.

36 MATERIALS SCIENCE↗
DOE OSTI2015

In Situ Localized Surface Plasmon Resonance (LSPR) Spectroscopy to Investigate Kinetics of Chemical Bath Deposition of CdS Thin Films

Techniques that can characterize the early stages of thin film deposition from liquid phase processes can aid greatly in our understanding of mechanistic aspects of chemical bath deposition (CBD). Here we have used localized surface plasmon resonance (LSPR) spectroscopy to monitor in-situ the kinetics of early-stage growth of cadmium sulfide (CdS) thin films on Ag nanoparticle on quartz substrates. Real-time shift during CdS deposition showed that the LSPR wavelength red shifted rapidly due to random deposition of CdS on the substrate, but saturated at longer times. LSPR modeling showed that these features could be interpreted as an initial deposition of CdS islands followed by preferential deposition onto itself. The CdS also showed significantly enhanced Raman signals up to 170 times due to surface enhanced raman scattering (SERS) from the CdS/Ag NP regions. The ex-situ SERS effect supported the LSPR shift suggesting that these techniques could be used to understand nucleation and growth phenomena from the liquid phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Direct observation of localized surface plasmon field enhancement by Kelvin probe force microscopy

A surface plasmon (SP) is a fundamental excitation state that exists in metal nanostructures. Over the past several years, the performance of optoelectronic devices has been improved greatly via the SP enhancement effect. In our previous work, the responsivity of GaN ultraviolet detectors was increased by over 30 times when using Ag nanoparticles. However, the physics of the SP enhancement effect has not been established definitely because of the lack of experimental evidence. To reveal the physical origin of this enhancement, Kelvin probe force microscopy (KPFM) was used to observe the SP-induced surface potential reduction in the vicinity of Ag nanoparticles on a GaN epilayer. Under ultraviolet illumination, the localized field enhancement induced by the SP forces the photogenerated electrons to drift close to the Ag nanoparticles, leading to a reduction of the surface potential around the Ag nanoparticles on the GaN epilayer. For an isolated Ag nanoparticle with a diameter of ~200 nm, the distribution of the SP localized field is located within 60 nm of the boundary of the Ag nanoparticle. For a dimer of Ag nanoparticles, the localized field enhancement between the nanoparticles was the strongest. The results presented here provide direct experimental proof of the localized field enhancement. In conclusion, these results not only explain the high performance of GaN detectors observed with the use of Ag nanoparticles but also reveal the physical mechanism of SP enhancement in optoelectronic devices, which will help us further understand and improve the performance of SP-based optoelectronic devices in the future.

36 MATERIALS SCIENCE↗
DOE OSTI2016

High-contrast and fast electrochromic switching enabled by plasmonics

With vibrant colours and simple, room-temperature processing methods, electrochromic polymers have attracted attention as active materials for flexible, low-power-consuming devices. However, slow switching speeds in devices realized to date, as well as the complexity of having to combine several distinct polymers to achieve a full-colour gamut, have limited electrochromic materials to niche applications. Here we achieve fast, high-contrast electrochromic switching by significantly enhancing the interaction of light—propagating as deep-subwavelength-confined surface plasmon polaritons through arrays of metallic nanoslits, with an electrochromic polymer—present as an ultra-thin coating on the slit sidewalls. The switchable configuration retains the short temporal charge-diffusion characteristics of thin electrochromic films, while maintaining the high optical contrast associated with thicker electrochromic coatings. In conclusion, we further demonstrate that by controlling the pitch of the nanoslit arrays, it is possible to achieve a full-colour response with high contrast and fast switching speeds, while relying on just one electrochromic polymer.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Probing topological protection using a designer surface plasmon structure

Topological photonic states, inspired by robust chiral edge states in topological insulators, have recently been demonstrated in a few photonic systems, including an array of coupled on-chip ring resonators at communication wavelengths. However, the intrinsic difference between electrons and photons determines that the 'topological protection' in time-reversal-invariant photonic systems does not share the same robustness as its counterpart in electronic topological insulators. Here in a designer surface plasmon platform consisting of tunable metallic sub-wavelength structures, we construct photonic topological edge states and probe their robustness against a variety of defect classes, including some common time-reversal-invariant photonic defects that can break the topological protection, but do not exist in electronic topological insulators. Furthermore, this is also an experimental realization of anomalous Floquet topological edge states, whose topological phase cannot be predicted by the usual Chern number topological invariants.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Product selectivity in plasmonic photocatalysis for carbon dioxide hydrogenation

Photocatalysis has not found widespread industrial adoption, in spite of decades of active research, because the challenges associated with catalyst illumination and turnover outweigh the touted advantages of replacing heat with light. A demonstration that light can control product selectivity in complex chemical reactions could prove to be transformative. Here, we show how the recently demonstrated plasmonic behaviour of rhodium nanoparticles profoundly improves their already excellent catalytic properties by simultaneously reducing the activation energy and selectively producing a desired but kinetically unfavourable product for the important carbon dioxide hydrogenation reaction. Methane is almost exclusively produced when rhodium nanoparticles are mildly illuminated as hot electrons are injected into the anti-bonding orbital of a critical intermediate, while carbon monoxide and methane are equally produced without illumination. As a result, the reduced activation energy and super-linear dependence on light intensity cause the unheated photocatalytic methane production rate to exceed the thermocatalytic rate at 350°C.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Electronic modulation of infrared radiation in graphene plasmonic resonators

All matter at finite temperatures emits electromagnetic radiation due to the thermally induced motion of particles and quasiparticles. Dynamic control of this radiation could enable the design of novel infrared sources; however, the spectral characteristics of the radiated power are dictated by the electromagnetic energy density and emissivity, which are ordinarily fixed properties of the material and temperature. Here we experimentally demonstrate tunable electronic control of blackbody emission from graphene plasmonic resonators on a silicon nitride substrate. It is shown that the graphene resonators produce antenna-coupled blackbody radiation, which manifests as narrow spectral emission peaks in the mid-infrared. By continuously varying the nanoresonator carrier density, the frequency and intensity of these spectral features can be modulated via an electrostatic gate. This work opens the door for future devices that may control blackbody radiation at timescales beyond the limits of conventional thermo-optic modulation.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Tracing terahertz plasmon polaritons with a tunable-by-design dispersion in topological insulator metaelements

Abstract Collective oscillations of massless charge carriers in two-dimensional materials—Dirac plasmon polaritons (DPPs)—are of paramount importance for engineering nanophotonic devices with tunable optical response. However, tailoring the optical properties of DPPs in a nanomaterial is a very challenging task, particularly at terahertz (THz) frequencies, where the DPP momentum is more than one order of magnitude larger than that of the free-space photons, and DDP attenuation is high. Here, we conceive and demonstrate a strategy to tune the DPP dispersion in topological insulator metamaterials. We engineer laterally coupled linear metaelements, fabricated from epitaxial Bi 2 Se 3, with selected coupling distances with the purpose to tune their wavevector, by geometry. We launch and directly map the propagation of DPPs confined within coupled meta-atoms via phase-sensitive scattering-type scanning near-field nanoscopy. We demonstrate that the DPP wavelength can be tuned by varying the metaelements coupling distance, resulting in up to a 20% increase of the polariton wavevector Re(k p ) in dimers and triplets with a 1 μm spacing, with reduced losses and a >50% increase of the polariton attenuation length.

Optics↗
DOE OSTI2017

Dynamically controlled Purcell enhancement of visible spontaneous emission in a gated plasmonic heterostructure

Emission control of colloidal quantum dots (QDs) is a cornerstone of modern high-quality lighting and display technologies. Dynamic emission control of colloidal QDs in an optoelectronic device is usually achieved by changing the optical pump intensity or injection current density. Here we propose and demonstrate a distinctly different mechanism for the temporal modulation of QD emission intensity at constant optical pumping rate. Our mechanism is based on the electrically controlled modulation of the local density of optical states (LDOS) at the position of the QDs, resulting in the modulation of the QD spontaneous emission rate, far-field emission intensity, and quantum yield. We manipulate the LDOS via field effect-induced optical permittivity modulation of an ultrathin titanium nitride (TiN) film, which is incorporated in a gated TiN/SiO 2 /Ag plasmonic heterostructure. In conclusion, the demonstrated electrical control of the colloidal QD emission provides a new approach for modulating intensity of light in displays and other optoelectronics.

42 ENGINEERING↗
DOE OSTI2017

Zero-field edge plasmons in a magnetic topological insulator [Zero-field edge magnetoplasmons in a magnetic topological insulator]

Incorporating ferromagnetic dopants into three-dimensional topological insulator thin films has recently led to the realisation of the quantum anomalous Hall effect. These materials are of great interest since they may support electrical currents that flow without resistance, even at zero magnetic field. To date, the quantum anomalous Hall effect has been investigated using low-frequency transport measurements. However, transport results can be difficult to interpret due to the presence of parallel conductive paths, or because additional non-chiral edge channels may exist. Here we move beyond transport measurements by probing the microwave response of a magnetised disk of Cr-(Bi,Sb) 2 Te 3 . We identify features associated with chiral edge plasmons, a signature that robust edge channels are intrinsic to this material system. Finally, our results provide a measure of the velocity of edge excitations without contacting the sample, and pave the way for an on-chip circuit element of practical importance: the zero-field microwave circulator.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗