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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 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

All-optical switching of an epsilon-near-zero plasmon resonance in indium tin oxide

Abstract Nonlinear optical devices and their implementation into modern nanophotonic architectures are constrained by their usually moderate nonlinear response. Recently, epsilon-near-zero (ENZ) materials have been found to have a strong optical nonlinearity, which can be enhanced through the use of cavities or nano-structuring. Here, we study the pump dependent properties of the plasmon resonance in the ENZ region in a thin layer of indium tin oxide (ITO). Exciting this mode using the Kretschmann-Raether configuration, we study reflection switching properties of a 60 nm layer close to the resonant plasmon frequency. We demonstrate a thermal switching mechanism, which results in a shift in the plasmon resonance frequency of 20 THz for a TM pump intensity of 70 GW cm −2 . For degenerate pump and probe frequencies, we highlight an additional two-beam coupling contribution, not previously isolated in ENZ nonlinear optics studies, which leads to an overall pump induced change in reflection from 1% to 45%.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Non-thermal emission in gap-mode plasmon photoluminescence

Abstract Photoluminescence from spatially inhomogeneous plasmonic nanostructures exhibits fascinating wavelength-dependent nonlinear behaviors due to the intraband recombination of hot electrons excited into the conduction band of the metal. The properties of the excited carrier distribution and the role of localized plasmonic modes are subjects of debate. In this work, we use plasmonic gap-mode resonators with precise nanometer-scale confinement to show that the nonlinear photoluminescence behavior can become dominated by non-thermal contributions produced by the excited carrier population that strongly deviates from the Fermi-Dirac distribution due to the confinement-induced large-momentum free carrier absorption beyond the dipole approximation. These findings open new pathways for controllable light conversion using nonequilibrium electron states at the nanoscale.

Science & Technology - Other Topics↗
DOE OSTI2026

Imaging a terahertz superfluid plasmon in a two-dimensional superconductor

The superconducting gap defines the fundamental energy scale for the emergence of dissipationless transport and collective phenomena in a superconductor. In layered high-temperature cuprate superconductors, in which the Cooper pairs are confined to weakly coupled two-dimensional (2D) copper–oxygen (CuO 2 ) planes, terahertz (THz) spectroscopy at subgap millielectronvolt (meV) energies has provided crucial insights into the collective superfluid response perpendicular to the superconducting layers. However, within the CuO 2 planes, the collective superfluid response manifests as plasmonic charge oscillations at energies far exceeding the superconducting gap, obscured by strong dissipation. Here, in this study, we present spectroscopic evidence of a below-gap, 2D superfluid plasmon in few-layer Bi 2 Sr 2 CaCu 2 O 8+x and spatially resolve its deeply subdiffractive THz electrodynamics. By placing the superconductor in the near field of a spintronic THz emitter, we reveal this distinct resonance—absent in bulk samples and observed only in the superconducting phase—and determine its plasmonic nature by mapping the geometric anisotropy and dispersion. Crucially, these measurements offer a direct view of the momentum-dependent and frequency-dependent superconducting transition in two dimensions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Plasmon induced modification of silicon nanocrystals photoluminescence in presence of gold nanostripes

Here, we report on the results of theoretical and experimental studies of photoluminescense of silicon nanocrystals in the proximity to plasmonic modes of different types. In the studied samples, the type of plasmonic mode is determined by the filling ratio of a one-dimensional array of gold stripes which covers the thin film with silicon nanocrystals on a quartz substrate. We analyze the extinction, photoluminesce spectra and decay kinetics of silicon nanocrystals and show that the incident and emitted light is coupled to the corresponding plasmonic mode. We demonstrate the modification of the extinction and photoluminesce spectra under the transition from wide to narrow gold stripes. The experimental extinction and photoluminescense spectra are in good agreement with theoretical calculations performed by the rigorous coupled wave analysis. Finally, we study the contribution of individual silicon nanocrystals to the overall photoluminescense intensity, depending on their spacial position inside the structure.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Visualizing the bidirectional optical transfer function for near-field enhancement in waveguide coupled plasmonic transducers

Here, we report visualizations of the bidirectional near-field optical transfer function for a waveguide-coupled plasmonic transducer as a metrology technique essential for successful development for mass-fabricated near-field devices. Plasmonic devices have revolutionized the observation of nanoscale phenomena, enabling optical excitation and readout from nanoscale regions of fabricated devices instead of as limited by optical diffraction. Visualizations of the plasmonic transducer modes were acquired both by local near-field excitation of the antenna on the front facet of a waveguide using the focused electron beam of a scanning electron microscope as a probe of the near-field cathodoluminescence during far-field collection from the back facet of the waveguide, and by local mapping of the optical near-field for the same antenna design using scattering scanning near-field optical microscopy as a probe of the near-field optical mode density for far-field light focused into the back facet of the waveguide. Strong agreement between both measurement types and numerical modeling was observed, indicating that the method enables crucial metrological comparisons of as fabricated device performance to as-modeled device expectations for heat-assisted magnetic recording heads, which can be extended to successful development of future near-field-on-chip devices such as optical processor interconnects.

42 ENGINEERING↗
DOE OSTI2016

Nanoscale mapping of plasmon and exciton in ZnO tetrapods coupled with Au nanoparticles

Metallic nanoparticles can be used to enhance optical absorption or emission in semiconductors, thanks to a strong interaction of collective excitations of free charges (plasmons) with electromagnetic fields. Herein we present direct imaging at the nanoscale of plasmon-exciton coupling in Au/ZnO nanostructures by combining scanning transmission electron energy loss and cathodoluminescence spectroscopy and mapping. The Au nanoparticles (~30 nm in diameter) are grown in-situ on ZnO nanotetrapods by means of a photochemical process without the need of binding agents or capping molecules, resulting in clean interfaces. Interestingly, the Au plasmon resonance is localized at the Au/vacuum interface, rather than presenting an isotropic distribution around the nanoparticle. Moreover, on the contrary, a localization of the ZnO signal has been observed inside the Au nanoparticle, as also confirmed by numerical simulations.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2016

Visualizing Surface Plasmons with Photons, Photoelectrons, and Electrons

Both photons and electrons may be used to excite surface plasmon polaritons, the collective charge density fluctuations at the surface of metal nanostructures. By virtue of their nanoscopic and dissipative nature, a detailed characterization of surface plasmon (SP) eigenmodes in real space-time ultimately requires joint sub-nanometer spatial and sub-femtosecond temporal resolution. The latter realization has driven significant developments in the past few years, aimed at interrogating both localized and propagating SP modes over the relevant length and time scales. In this mini-review, we briefly highlight different techniques we employ to visualize the enhanced electric fields associated with SPs. Specifically, we discuss recent hyperspectral optical microscopy, tip-enhanced Raman nano-spectroscopy, nonlinear photoemission electron microscopy, as well as correlated scanning transmission electron microscopy-electron energy loss spectroscopy measurements targeting prototypical plasmonic nanostructures and constructs. Through selected practical examples, we examine the information content in multidimensional images recorded by taking advantage of each of the aforementioned techniques. In effect, we illustrate how SPs can be visualized at the ultimate limits of space and time.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2017

Intermediate selectivity in the oxidation of phenols using plasmonic Au/ZnO photocatalysts

Tunable reaction selectivity on a single catalyst is a continual goal in chemical syntheses. Herein, we report an unexpected light-directed intermediate selectivity using well-known plasmonic photocatalysts. We observed distinct intermediate selectivity behaviors between using UV and visible light irradiations. Chemical computations and quenching experiments suggest that the radicals generated by the plasmonic excitation govern the light-directed selectivity. As a result, the broader impact of this work ranges from selective yield of desirable intermediates for subsequent syntheses without tedious separation procedures, to arousing interest in examining new opportunities for plasmonic photocatalysts.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Understanding plasmon coupling in nanoparticle dimers using molecular orbitals and configuration interaction

Here, we perform a theoretical investigation of the electronic structure and optical properties of atomic nanowire and nanorod dimers using DFT and TDDFT. In both systems at separation distances larger than 0.75 nm, optical spectra show a single feature that resembles the bonding dipole plasmon (BDP) mode. A configuration interaction (CI) analysis shows that the BDP mode arises from constructive coupling of transitions, whereas the destructive coupling does not produce significant oscillator strength for such separation distances. At shorter separation distances, both constructive and destructive coupling produce oscillator strength due to wave-function overlap, which results in multiple features in the calculated spectra. Our analysis shows that a charge-transfer plasmon (CTP) mode arises from destructive coupling of transitions, whereas the BDP results from constructive coupling of the same transitions at shorter separation distances. Furthermore, the coupling elements between these transitions are shown to depend heavily on the amount of exact Hartree–Fock exchange (HFX) in the functional, which affects the splitting of CTP and BDP modes. With 50% HFX or more, the CTP and BDP modes mainly merge into a single feature in the spectra. These findings suggest that the effects of exact exchange must be assessed during the prediction of CTP modes in plasmonic systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Ultrafast relaxation dynamics in bimetallic plasmonic catalysts

Combining a plasmonic metal, such as gold, with other popular catalysts, such as Ni or Pt, can extend its benefits to many energy-extensive reactions catalyzed by those metals. The efficiency of a plasmon-enhanced catalytic reaction is mainly determined by the light absorption cross section and the photoexcited charge carrier relaxation dynamics of the nanoparticles. Here we have investigated the charge carrier relaxation dynamics of gold/nickel (Au/Ni) and gold/platinum (Au/Pt) bimetallic nanoparticles. We found that the addition of Ni or Pt to gold can reduce light absorption in gold nanoparticles. However, electron–phonon coupling rates of Au/Ni and Au/Pt nanoparticles are significantly faster than that of pure Au nanoparticles. This is due to the fact that both Ni and Pt possess significantly larger electron–phonon coupling constants and higher densities of states near the Fermi level in comparison with Au. Additionally, the phonon–phonon coupling rate of bimetallic Au/Pt and Au/Ni nanoparticles was significantly different from that of pure gold nanoparticles, due to the acoustic impedance mismatch at the nanoparticle/substrate interface. Our findings provide important insights into the rational design of bimetallic plasmonic catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Design-controlled synthesis of IrO 2 sub-monolayers on Au nanoflowers: marrying plasmonic and electrocatalytic properties

We develop herein plasmonic–catalytic Au–IrO 2 nanostructures with a morphology optimized for efficient light harvesting and catalytic surface area; the nanoparticles have a nanoflower morphology, with closely spaced Au branches all partially covered by an ultrathin (1 nm) IrO 2 shell. This nanoparticle architecture optimizes optical features due to the interactions of closely spaced plasmonic branches forming electromagnetic hot spots, and the ultra-thin IrO 2 layer maximizes efficient use of this expensive catalyst. This concept was evaluated towards the enhancement of the electrocatalytic performances towards the oxygen evolution reaction (OER) as a model transformation. The OER can play a central role in meeting future energy demands but the performance of conventional electrocatalysts in this reaction is limited by the sluggish OER kinetics. We demonstrate an improvement of the OER performance for one of the most active OER catalysts, IrO 2 , by harvesting plasmonic effects from visible light illumination in multimetallic nanoparticles. We find that the OER activity for the Au–IrO 2 nanoflowers can be improved under LSPR excitation, matching best properties reported in the literature. Our simulations and electrocatalytic data demonstrate that the enhancement in OER activities can be attributed to an electronic interaction between Au and IrO 2 and to the activation of Ir–O bonds by LSPR excited hot holes, leading to a change in the reaction mechanism (rate-determinant step) under visible light illumination.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

A versatile strategy for controlled assembly of plasmonic metal/semiconductor hemispherical nano-heterostructure arrays

Recent advances in manipulating plasmonic properties of metal/semiconductor heterostructures have opened up new avenues for basic research and applications. Herein, we present a versatile strategy for the assembly of arrays of plasmonic metal/semiconductor hemispherical nano-heterostructures (MSHNs) with control over spacing and size of the metal/semiconductor heterostructure array, which can facilitate a wide range of scientific studies and applications. The strategy combines nanosphere lithography for generating the metal core array with solution-based chemical methods for the semiconductor shell that are widely available and kinetically controllable. Periodic arrays of Au/Cu 2 O and Ag/Cu 2 O heterostructures are synthesized to demonstrate the approach and highlight the versatility and importance of the tunability of plasmonic properties. The morphology, structure, optical properties, and elemental compositions of the heterostructures were analyzed. Finally, this strategy can be important for understanding and manipulating fundamental nanoscale solid-state physical and chemical properties, as well as assembling heterostructures with desirable structure and functionality for applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Plasmonic behavior of gold nanorod heterodimers with free-electron feed

The plasmon coupling between metal nanostructures can lead to huge local electric field enhancement and new plasmon modes. Here, we study the effect of the close proximity of two gold nanorod particles on the modification of localized surface plasmon (LSP) modes of the individual on gold nanorod in spectral and spatial domain using cathodoluminescence (CL) spectroscopy and imaging in a high resolution scanning electron microscope (SEM). Significantly enhanced resonant emission is observed from the nanorod dimers when the electron beam is injected around the junction between the rods, where the local density of electromagnetic states is raised.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Resonant quantum efficiency enhancement of midwave infrared nBn photodetectors using one-dimensional plasmonic gratings

We demonstrate up to 39% resonant enhancement of the quantum efficiency (QE) of a low dark current nBn midwave infrared photodetector with a 0.5 μm InAsSb absorber layer. The enhancement was achieved by using a 1D plasmonic grating to couple incident light into plasmon modes propagating in the plane of the device. The plasmonic grating is composed of stripes of deposited amorphous germanium overlaid with gold. Devices with and without gratings were processed side-by-side for comparison of their QEs and dark currents. The peak external QE for a grating device was 29% compared to 22% for a mirror device when the illumination was polarized perpendicularly to the grating lines. Additional experiments determined the grating coupling efficiency by measuring the reflectance of analogous gratings deposited on bare GaSb substrates.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Enhanced photoluminescence of Si nanocrystals-doped cellulose nanofibers by plasmonic light scattering

We report the development of bio-compatible cellulose nanofibers doped with light emitting silicon nanocrystals and Au nanoparticles via facile electrospinning. By performing photoluminescence (PL) spectroscopy as a function of excitation wavelength, we demonstrate plasmon-enhanced PL by a factor of 2.2 with negligible non-radiative quenching due to plasmon-enhanced scattering of excitation light from Au nanoparticles to silicon nanocrystals inside the nanofibers. These findings provide an alternative approach for the development of plasmon-enhanced active systems integrated within the compact nanofiber geometry. Furthermore, bio-compatible light-emitting nanofibers prepared by a cost-effective solution-based processing are very promising platforms for biophotonic applications such as fluorescence sensing and imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Plasmon-induced dynamics of H{sub 2} splitting on a silver atomic chain

Localized surface plasmon resonances (LSPR) supported in metal nanostructures can be efficiently harnessed to drive photocatalytic reactions, whose atomic scale mechanism remains a challenge. Here, real-time dynamics of H{sub 2} photosplitting on a linear silver atomic chain, upon exposure to femtosecond laser pulses, has been investigated using time-dependent density functional theory. The wavelength dependent H{sub 2} splitting process is strongly coupled to LSPR excitation in silver chain. We identify that hot electrons produced in the silver chain by plasmon excitation are transferred to the antibonding state of the adsorbed H{sub 2} and trigger H{sub 2} dissociation, consistent with experimental observations. Increasing illumination intensity and the length of atomic chain promote H{sub 2} splitting, thanks to stronger LSPR. Dynamic electronic response can be quantitatively described within the present approach, providing insights towards a complete fundamental understanding on plasmon-induced chemical reactions at the microscopic scale.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Double-shelled plasmonic Ag-TiO{sub 2} hollow spheres toward visible light-active photocatalytic conversion of CO{sub 2} into solar fuel

Double-shelled hollow hybrid spheres consisting of plasmonic Ag and TiO{sub 2} nanoparticles were successfully synthesized through a simple reaction process. The analysis reveals that Ag nanoparticles were dispersed uniformly in the TiO{sub 2} nanoparticle shell. The plasmonic Ag-TiO{sub 2} hollow sphere proves to greatly enhance the photocatalytic activity toward reduction of CO{sub 2} into renewable hydrocarbon fuel (CH{sub 4}) in the presence of water vapor under visible-light irradiation. The possible formation mechanism of the hollow sphere and related plasmon-enhanced photocatalytic performance were also briefly discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Resonance hybridization and near field properties of strongly coupled plasmonic ring dimer-rod nanosystem

Combined effects of polarization, split gap, and rod width on the resonance hybridization and near field properties of strongly coupled gold dimer-rod nanosystem are comparatively investigated in the light of the constituent nanostructures. By aligning polarization of the incident light parallel to the long axis of the nanorod, introducing small split gaps to the dimer walls, and varying width of the nanorod, we have simultaneously achieved resonance mode coupling, huge near field enhancement, and prolonged plasmon lifetime. As a result of strong coupling between the nanostructures and due to an intense confinement of near fields at the split and dimer-rod gaps, the extinction spectrum of the coupled nanosystem shows an increase in intensity and blueshift in wavelength. Consequently, the near field lifespan of the split-nanosystem is prolonged in contrast to the constituent nanostructures and unsplit-nanosystem. On the other hand, for polarization of the light perpendicular to the long axis of the nanorod, the effect of split gap on the optical responses of the coupled nanosystem is found to be insignificant compared to the parallel polarization. These findings and such geometries suggest that coupling an array of metallic split-ring dimer with long nanorod can resolve the huge radiative loss problem of plasmonic waveguide. In addition, the Fano-like resonances and immense near field enhancements at the split and dimer-rod gaps imply the potentials of the nanosystem for practical applications in localized surface plasmon resonance spectroscopy and sensing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗