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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 667 records · Page 37
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Theory and computation of hot carriers generated by surface plasmon polaritons in noble metals

Hot carriers (HC) generated by surface plasmon polaritons (SPPs) in noble metals are promising for application in optoelectronics, plasmonics and renewable energy. However, existing models fail to explain key quantitative details of SPP-to-HC conversion experiments. Here we develop a quantum mechanical framework and apply first-principles calculations to study the energy distribution and scattering processes of HCs generated by SPPs in Au and Ag. We find that the relative positions of the s and d bands of noble metals regulate the energy distribution and mean free path of the HCs, and that the electron–phonon interaction controls HC energy loss and transport. Our results prescribe optimal conditions for HC generation and extraction, and invalidate previously employed free-electron-like models. Our work combines density functional theory, GW and electron–phonon calculations to provide microscopic insight into HC generation and ultrafast dynamics in noble metals.

ultrafast photonics↗
DOE OSTI2016

Nanoscale form dictates mesoscale function in plasmonic DNA–nanoparticle superlattices

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.

Ross, Michael B.↗
DOE OSTI2017

Band-edge engineering for controlled multi-modal nanolasing in plasmonic superlattices

Single band-edge states can trap light and function as high-quality optical feedback for microscale lasers and nanolasers. However, access to more than a single band-edge mode for nanolasing has not been possible because of limited cavity designs. Here, we describe how plasmonic superlattices-finite-arrays of nanoparticles (patches) grouped into microscale arrays-can support multiple band-edge modes capable of multi-modal nanolasing at programmed emission wavelengths and with large mode spacings. Different lasing modes show distinct input-output light behaviour and decay dynamics that can be tailored by nanoparticle size. By modelling the superlattice nanolasers with a four-level gain system and a time-domain approach, we reveal that the accumulation of population inversion at plasmonic hot spots can be spatially modulated by the diffractive coupling order of the patches. Furthermore, we show that symmetry-broken superlattices can sustain switchable nanolasing between a single mode and multiple modes.

42 ENGINEERING↗
DOE OSTI2020

Ten years of spasers and plasmonic nanolasers

Ten years ago, three teams experimentally demonstrated the first spasers, or plasmonic nanolasers, after the spaser concept was first proposed theoretically in 2003. An overview of the significant progress achieved over the last 10 years is presented here, together with the original context of and motivations for this research. After a general introduction, we first summarize the fundamental properties of spasers and discuss the major motivations that led to the first demonstrations of spasers and nanolasers. This is followed by an overview of crucial technological progress, including lasing threshold reduction, dynamic modulation, room-temperature operation, electrical injection, the control and improvement of spasers, the array operation of spasers, and selected applications of single-particle spasers. Research prospects are presented in relation to several directions of development, including further miniaturization, the relationship with Bose–Einstein condensation, novel spaser-based interconnects, and other features of spasers and plasmonic lasers that have yet to be realized or challenges that are still to be overcome.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Enhanced generation and anisotropic Coulomb scattering of hot electrons in an ultra-broadband plasmonic nanopatch metasurface

The creation of energetic electrons through plasmon excitation of nanostructures before thermalization has been proposed for a wide number of applications in optical energy conversion and ultrafast nanophotonics. However, the use of "nonthermal" electrons is primarily limited by both a low generation efficiency and their ultrafast decay. We report experimental and theoretical results on the use of broadband plasmonic nanopatch metasurfaces comprising a gold substrate coupled to silver nanocubes that produce large concentrations of hot electrons, which we measure using transient absorption spectroscopy. We find evidence for three subpopulations of nonthermal carriers which we propose arise from anisotropic electron-electron scattering within sp-bands near the Fermi surface. The bimetallic character of the metasurface strongly impacts the physics, with dissipation occurring primarily in the gold whereas the quantum process of hot electron generation takes place in both components. As a result, our calculations show that the choice of geometry and materials is crucial for producing strong ultrafast nonthermal electron components.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Surface plasmons induce topological transition in graphene/α-MoO3 heterostructures

Abstract Polaritons in hyperbolic van der Waals materials—where principal axes have permittivities of opposite signs—are light-matter modes with unique properties and promising applications. Isofrequency contours of hyperbolic polaritons may undergo topological transitions from open hyperbolas to closed ellipse-like curves, prompting an abrupt change in physical properties. Electronically-tunable topological transitions are especially desirable for future integrated technologies but have yet to be demonstrated. In this work, we present a doping-induced topological transition effected by plasmon-phonon hybridization in graphene/α-MoO 3 heterostructures. Scanning near-field optical microscopy was used to image hybrid polaritons in graphene/α-MoO 3 . We demonstrate the topological transition and characterize hybrid modes, which can be tuned from surface waves to bulk waveguide modes, traversing an exceptional point arising from the anisotropic plasmon-phonon coupling. Graphene/α-MoO 3 heterostructures offer the possibility to explore dynamical topological transitions and directional coupling that could inspire new nanophotonic and quantum devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Observation of interlayer plasmon polaron in graphene/WS 2 heterostructures

Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get “dressed", which leads to the formation of polaronic quasiparticles. The exploration of polaronic effects on low-energy excitations is in its infancy in two-dimensional materials. Here, we present the discovery of an interlayer plasmon polaron in heterostructures composed of graphene on top of single-layer WS 2 . By using micro-focused angle-resolved photoemission spectroscopy during in situ doping of the top graphene layer, we observe a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the single-layer WS 2 conduction band minimum. Our results are explained by an effective many-body model in terms of a coupling between single-layer WS 2 conduction electrons and an interlayer plasmon mode. It is important to take into account the presence of such interlayer collective modes, as they have profound consequences for the electronic and optical properties of heterostructures that are routinely explored in many device architectures involving 2D transition metal dichalcogenides.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Plasmonic photoconductive terahertz focal-plane array with pixel super-resolution

Abstract Imaging systems operating in the terahertz part of the electromagnetic spectrum are attractive due to their ability to penetrate many opaque materials and provide unique spectral signatures of various chemicals. However, the use of terahertz imagers in real-world applications has been limited by the slow speed, large size, high cost and complexity of present systems, largely due to the lack of suitable terahertz focal-plane array detectors. Here we report a terahertz focal-plane array that can directly provide the spatial amplitude and phase distributions, along with the ultrafast temporal and spectral information of an imaged object. It consists of a two-dimensional array of ~0.3 million plasmonic photoconductive nanoantennas optimized to rapidly detect broadband terahertz radiation with a high signal-to-noise ratio. We utilized the multispectral nature of the amplitude and phase data captured by these plasmonic nanoantennas to image different objects, including super-resolved etched patterns in a silicon substrate and defects in battery electrodes. By eliminating the need for raster scanning and spatial terahertz modulation, our terahertz focal-plane array offers more than a 1,000-fold increase in the imaging speed compared with the state of the art and potentially suits a broad range of applications in industrial inspection, security screening and medical diagnosis, among others.

Optics↗
DOE OSTI2023

Pines’ demon observed as a 3D acoustic plasmon in Sr2RuO4

Abstract The characteristic excitation of a metal is its plasmon, which is a quantized collective oscillation of its electron density. In 1956, David Pines predicted that a distinct type of plasmon, dubbed a ‘demon’, could exist in three-dimensional (3D) metals containing more than one species of charge carrier 1 . Consisting of out-of-phase movement of electrons in different bands, demons are acoustic, electrically neutral and do not couple to light, so have never been detected in an equilibrium, 3D metal. Nevertheless, demons are believed to be critical for diverse phenomena including phase transitions in mixed-valence semimetals 2 , optical properties of metal nanoparticles 3 , soundarons in Weyl semimetals 4 and high-temperature superconductivity in, for example, metal hydrides 3,5–7 . Here, we present evidence for a demon in Sr 2 RuO 4 from momentum-resolved electron energy-loss spectroscopy. Formed of electrons in the β and γ bands, the demon is gapless with critical momentum q c = 0.08 reciprocal lattice units and room-temperature velocity v = (1.065 ± 0.12) × 10 5 m s −1 that undergoes a 31% renormalization upon cooling to 30 K because of coupling to the particle–hole continuum. The momentum dependence of the intensity of the demon confirms its neutral character. Our study confirms a 67-year old prediction and indicates that demons may be a pervasive feature of multiband metals.

Science & Technology - Other Topics↗
DOE OSTI2017

Broadband polarization conversion with anisotropic plasmonic metasurfaces

Metasurfaces offer exciting opportunities that enable precise control of light propagation, optical intensity, phase and polarization. Plasmonic metasurface based quarter-wave plates have been recently studied to realize the conversion between linear polarization and circular polarization. However, it is still quite challenging to directly measure the birefringent phase retardation introduced by metasurface wave plates with a reliable technique. Here, we report a high-performance broadband metasurface quarter-wave plate made of anisotropic T-shaped plasmonic antennas in near-infrared wavelength range, where the achromatic nearly 90° transmitted phase retardation through the metasurface is precisely characterized with an optical vortex based interferometric approach. Based on the measured transmission amplitude and phase of two orthogonal linear polarization components, nearly unit degree of linear polarization is extracted from the Stokes parameters, indicating excellent broadband polarization conversion between linearly and circularly polarized light through the metasurface. Our results will be an important step forward in the advancement of integrated metasurface devices for polarization conversion and beam manipulation, structured light control, as well as new spectroscopic and interferometric techniques for metasurface characterization.

Science & Technology - Other Topics↗
DOE OSTI2015

Super-resolution of fluorescence-free plasmonic nanoparticles using enhanced dark-field illumination based on wavelength-modulation

Super-resolution imaging of fluorescence-free plasmonic nanoparticles (NPs) was achieved using enhanced dark-field (EDF) illumination based on wavelength-modulation. Indistinguishable adjacent EDF images of 103-nm gold nanoparticles (GNPs), 40-nm gold nanorods (GNRs), and 80-nm silver nanoparticles (SNPs) were modulated at their wavelengths of specific localized surface plasmon scattering. The coordinates (x, y) of each NP were resolved by fitting their point spread functions with a two-dimensional Gaussian. The measured localization precisions of GNPs, GNRs, and SNPs were 2.5 nm, 5.0 nm, and 2.9 nm, respectively. From the resolved coordinates of NPs and the corresponding localization precisions, super-resolution images were reconstructed. Depending on the spontaneous polarization of GNR scattering, the orientation angle of GNRs in two-dimensions was resolved and provided more elaborate localization information. This novel fluorescence-free super-resolution method was applied to live HeLa cells to resolve NPs and provided remarkable subdiffraction limit images.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2015

Control of plasmonic nanoantennas by reversible metal-insulator transition

We demonstrate dynamic reversible switching of VO 2 insulator-to-metal transition (IMT) locally on the scale of 15 nm or less and control of nanoantennas, observed for the first time in the near-field. Using polarization-selective near-field imaging techniques, we simultaneously monitor the IMT in VO 2 and the change of plasmons on gold infrared nanoantennas. Structured nanodomains of the metallic VO 2 locally and reversibly transform infrared plasmonic dipole nanoantennas to monopole nanoantennas. Fundamentally, the IMT in VO 2 can be triggered on femtosecond timescale to allow ultrafast nanoscale control of optical phenomena. In conclusion, these unique features open up promising novel applications in active nanophotonics.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Photons, phonons, and plasmons with orbital angular momentum in plasmas

Exact eigen modes with orbital angular momentum (OAM) in the complex media of unmagnetized homogeneous plasmas are studied. Three exact eigen modes with OAM are derived, i.e., photons, phonons, and plasmons. The OAM of different plasma components are closely related to the charge polarities. For photons, the OAM of electrons and ions are of the same magnitude but opposite direction, and the total OAM is carried by the field. For the phonons and plasmons, their OAM are carried by the electrons and ions. Lastly, the OAM modes in plasmas and their characteristics can be explored for potential applications in plasma physics and accelerator physics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2018

Anisotropic ultraviolet-plasmon dispersion in black phosphorus

Via momentum-resolved electron energy loss spectroscopy (EELS) coupled with scanning transmission electron microscopy, we have studied the dispersion relation of interband plasmonic modes in the ultraviolet in black phosphorus. We find that the dispersion of the interband plasmons is anisotropic. Experimental results are reproduced by density functional theory, by taking into account both the anisotropy of the single-particle response function, arising from the anisotropic band structure, and the damping. Moreover, our theoretical model also indicates the presence of low-energy excitations in the near-infrared that are selectively active in the armchair direction, whose existence has been experimentally validated by high-resolution EELS (HREELS) in reflection mode.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Solvent-induced local environment effect in plasmonic catalysis

Solvents are known to affect the local surface plasmon resonance of metal nanoparticles; however, how solvents can be used to manipulate the interfacial charge and energy transfer in plasmonic catalysis remains to be explored.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Plasmon-induced charge separation at two-dimensional gold semishell arrays on SiO{sub 2}@TiO{sub 2} colloidal crystals

Photoelectrodes based on plasmonic Au semishell (or halfshell) arrays are developed. A colloidal crystal consisting of SiO{sub 2}@TiO{sub 2} core-shell particles is prepared on a TiO{sub 2}-coated transparent electrode. A Au semishell (or halfshell) array is deposited by sputtering or evaporation on the colloidal crystal. An electrode with the semishell (or halfshell) array exhibits negative photopotential shifts and anodic photocurrents under visible light at 500-800 nm wavelengths in an aqueous electrolyte containing an electron donor. In particular, hydroquinone and ethanol are good electron donors. The photocurrents can be explained in terms of plasmon-induced charge separation at the Au-TiO{sub 2} interface.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Particle shape inhomogeneity and plasmon-band broadening of solar-control LaB{sub 6} nanoparticles

An ensemble inhomogeneity of non-spherical LaB{sub 6} nanoparticles dispersion has been analyzed with Mie theory to account for the observed broad plasmon band. LaB{sub 6} particle shape has been characterized using small-angle X-ray scattering (SAXS) and electron tomography (ET). SAXS scattering intensity is found to vary exponentially with exponent −3.10, indicating the particle shape of disk toward sphere. ET analysis disclosed dually grouped distribution of nanoparticle dispersion; one is large-sized at small aspect ratio and the other is small-sized with scattered high aspect ratio, reflecting the dual fragmentation modes during the milling process. Mie extinction calculations have been integrated for 100 000 particles of varying aspect ratio, which were produced randomly by using the Box-Muller method. The Mie integration method has produced a broad and smooth absorption band expanded towards low energy, in remarkable agreement with experimental profiles by assuming a SAXS- and ET-derived shape distribution, i.e., a majority of disks with a little incorporation of rods and spheres for the ensemble. The analysis envisages a high potential of LaB{sub 6} with further-increased visible transparency and plasmon peak upon controlled particle-shape and its distribution.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗