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At least 595 records · Page 33

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DOE OSTI2016

Correlation of the plasmon-enhanced photoconductance and photovoltaic properties of core-shell Au@TiO{sub 2} network

This study reveals the contribution of hot electrons from the excited plasmonic nanoparticles in dye sensitized solar cells (DSSCs) by correlating the photoconductance of a core-shell Au@TiO{sub 2} network on a micro-gap electrode and the photovolatic properties of this material as photoanodes in DSSCs. The distinct wavelength dependence of these two devices reveals that the plasmon-excited hot electrons can easily overcome the Schottky barrier at Au/TiO{sub 2} interface in the whole visible wavelength range and transfer from Au nanoparticles into the TiO{sub 2} network. The enhanced charge carrier density leads to higher photoconductance and facilitates more efficient charge separation and photoelectron collection in the DSSCs.

36 MATERIALS SCIENCE↗

DOE OSTI2017

Surface plasmons and Bloch surface waves: Towards optimized ultra-sensitive optical sensors

In photonics, the field concentration and enhancement have been major objectives for achieving size reduction and device integration. Plasmonics offers resonant field confinement and enhancement, but ultra-sharp optical resonances in all-dielectric multi-layer thin films are emerging as a powerful contestant. Thus, applications capitalizing upon stronger and sharper optical resonances and larger field enhancements could be faced with a choice for the superior platform. Here in this paper, we present a comparison between plasmonic and dielectric multi-layer thin films for their resonance merits. We show that the remarkable characteristics of the resonance behavior of optimized dielectric multi-layers can outweigh those of their metallic counterpart.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Non-invasive low charge electron beam time-of-arrival diagnostic using a plasmonics-enhanced photoconductive antenna

The use of a plasmonics-enhanced photoconductive antenna (PCA) optically gated by a near infrared (NIR) pulse enables non-invasive time-of-arrival measurements of a low charge electron beam with respect to the NIR reference, achieving picosecond resolution. The measured signal values show the expected scaling with the beam charge and distance from PCA to the beam axis, as the PCA samples the electric field of the passing electron beam. We operate the device with an NIR spot size much larger than the PCA active-area, resulting in a very simple optical setup and alignment procedure, making the plasmonics-enhanced PCA a preferred alternative to more complex timing diagnostics for applications requiring non-invasive picosecond or sub-picosecond timestamping.

43 PARTICLE ACCELERATORS↗

DOE OSTI2019

Photonic thermal conduction by infrared plasmonic resonators in semiconductor nanowires

Photons typically do not contribute to thermal transport within a solid due to their low energy density and tendency to be absorbed quickly. In this article, we propose a practical material system—infrared plasmonic resonators embedded in a semiconductor nanowire—that leverages near-field electromagnetic coupling to achieve photonic thermal transport comparable to the electronic and phononic contributions. We analytically show photonic thermal conductivities up to about 1 W m -1 K -1 for 10 nm diameter Si and InAs nanowires containing repeated resonators at 500 K. Finally, the nanowire system outperforms plasmonic particles in isotropic environments and presents a pathway for photonic thermal transport to exceed that of phonons and electrons.

42 ENGINEERING↗

DOE OSTI2020

Non-Hermitian approach for quantum plasmonics

Herein, we examine the limits of applicability of a simple non-Hermitian model for exciton/plasmon interactions in the presence of dissipation and dephasing. The model can be used as an alternative to the more complete Lindblad density matrix approach and is computationally and conceptually simpler. We find that optical spectra in the linear regime can be adequately described by this approach. The model can fail, however, under continuous optical driving in some circumstances. In the case of two quantum dots or excitons interacting with a plasmon, the model can also describe coherences and entanglement qualitatively when both dissipation and dephasing are present and quantitatively in the limit with no dephasing. The approach, within a single excitation manifold, is also applied to assess the role of disorder for 50 quantum dots interacting with a plasmon, where we find that, on average, large enough disorder can help stabilize the ensemble average of the open quantum system toward a dark quasi-steady-state much faster than without disorder. Furthermore, while such single excitation manifold calculations in this size limit can readily be done with either the non-Hermitian or Lindblad forms, as one goes to larger Hilbert space sizes, the computational and storage advantages of the non-Hermitian approach can become more useful. Published under license by AIP Publishing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Observation of photo-induced plasmon–phonon coupling in PbTe via ultrafast x-ray scattering

We report the observation of photo-induced plasmon–phonon coupled modes in the group IV–VI semiconductor PbTe using ultrafast x-ray diffuse scattering at the Linac Coherent Light Source. We measure the near-zone-center excited-state dispersion of the heavily screened longitudinal optical (LO) phonon branch as extracted from differential changes in x-ray diffuse scattering intensity following above bandgap photoexcitation. We suggest that upon photoexcitation, the LO phonon-plasmon coupled (LOPC) modes themselves become coupled to longitudinal acoustic modes that drive electron band shifts via acoustic deformation potentials and possibly to low-energy single-particle excitations within the plasma and that these couplings give rise to displacement-correlations that oscillate in time with a period given effectively by the heavily screened LOPC frequency.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Enhancing hyperspectral EELS analysis of complex plasmonic nanostructures with pan-sharpening

Nanoscale hyperspectral techniques—such as electron energy loss spectroscopy (EELS)—are critical to understand the optical response in plasmonic nanostructures, but as systems become increasingly complex, the required sampling density and acquisition times become prohibitive for instrumental and specimen stability. As a result, there has been a recent push for new experimental methodologies that can provide comprehensive information about a complex system, while significantly reducing the duration of the experiment. In this work, we present a pan-sharpening approach to hyperspectral EELS analysis, where we acquire two datasets from the same region (one with high spatial resolution and one with high spectral fidelity) and combine them to achieve a single dataset with the beneficial properties of both. This work outlines a straightforward, reproducible pathway to reduced experiment times and higher signal-to-noise ratios, while retaining the relevant physical parameters of the plasmonic response, and is generally applicable to a wide range of spectroscopy modalities.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Superfocusing of an ultrashort plasmon pulse by a conducting cone

We have shown theoretically the possibility of controlling nanoscale superfocusing of plasmons in a metal conical tip by modulating the carrier frequency of the pulse. The propagation of an ultrashort plasmon pulse in a metal nanoneedle is simulated numerically. The calculation is based on an asymptotic analytical solution of Maxwell's equations for electromagnetic wave propagation in a conical conductor in the vicinity of its apex, obtained by the approximate separation of variables in spherical coordinates. The dependence the field superfocusing on the conductor material, pulse chirp and propagation length is studied. (nanooptics)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Amplification and generation of surface plasmon polaritons in a semiconductor film – dielectric structure

The peculiarities of propagation and amplification of surface waves of plasmon polariton type in a planar semiconductor film – dielectric structure are considered for the THz frequency region, with allowance for dissipation in a semiconductor. Two spectral regions are found, where the group velocity of surface plasmon polaritons is negative. It is shown that in these regions the structure can be considered as an amplifying waveguide with distributed feedback and a high gain with respect to the reflected and transmitted signals. The possibility of generation of electromagnetic radiation in such structures is established. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Continuous-wave laser generation of slow THz surface plasmons in an array of single-walled carbon nanotubes

The mechanism of generation of surface plasmon polaritons in the THz and far-IR ranges by laser irradiation of arrays of single-walled carbon nanotubes is considered. It is shown that by varying the angle of incidence of the laser beam, one can change the frequency of generated surface plasmon polaritons. As consequence, the nanotube length can be matched to the laser wavelength for efficient conversion of cw laser radiation to the THz range.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Conversion of light polarisation in asymmetric plasmonic waveguides

Hybrid plasmonic waveguides with an embedded conducting oxide layer can be used for producing fast and compact electro-optical modulation devices. However, due to constraints, which plasmon modes impose on light polarisation, modulators of this class are not compatible with high-efficiency modern diffraction gratings used for coupling light into a waveguide. In the present work we demonstrate how a simple structuring of a modulation sandwich makes it possible to produce a compact polarisation converter that eliminates the mentioned incompatibility. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2019

Localised plasmons in sphere-like fullerenes and nanoparticles with conducting shells: Classical electrodynamic approach

Based on the classical electrodynamic approach, we consider localised plasmons in fullerenes and small particles with metal layers and shells. At low energies of the radiation quantum, models of fullerenes as conducting shells are used taking into account the contribution of only π electrons, and at high energies, of both π and σ electrons. The obtained maxima of the scattering cross sections correspond to the values of 20 and 27 eV that were determined experimentally and in quantum models for the maxima of the photoionisation cross sections of fullerenes C{sub 60} and C{sub 28}, respectively. Approximate analytical results are presented for resonant frequencies, Q factors, radiation patterns, scattering and absorption cross sections for sphere-like particles and fullerenes, as well as integral equations and functionals for dielectric particles with a conducting shell of arbitrary shape. Analysis relies on the use of effective surface conductivity. (plasmons)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Design principles for photonic crystals based on plasmonic nanoparticle superlattices

Significance In this article, we derive a set of design principles for making photonic crystals with desired photonic stopband properties by taking advantage of spacer group, a design parameter enabled by recent advances in bottom-up assembly processes. The concept of spacer groups is experimentally realized through DNA-programmable assembly of Au nanoparticles, showing that highly reflective structures can be generated with cubic lattices and flexible spacer groups that can enable lighter and more compact 3D photonic crystals with precisely designed and even reconfigurable photonic properties. It also allows one to explore the combined effects of both photonic bandgap and the plasmonic properties of NPs, which may prove useful in fields spanning plasmonic cavity structures, optical nanocircuits, subwavelength imaging, and low-loss metamaterials.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Surface plasmon enhanced fast electron emission from metallised fibre optic nanotips

Physical mechanisms of electron emission from fibre optic nanotips, namely, tunnelling, multi-photon, and thermionic emission, either prevent fast switching or require intense laser fields. Time-resolved electron emission from nano-sized sources finds applications ranging from material characterisation to fundamental studies of quantum coherence. We present a nano-sized electron source capable of fast-switching (≤1 ns) that can be driven with low-power femtosecond lasers. The physical mechanism that can explain emission at low laser power is surface plasmon enhanced above-threshold photoemission. An electron emission peak is observed and provides support for resonant plasmonic excitation. The electron source is a metal-coated optical fibre tapered into a nano-sized tip. The fibre is flexible and back illuminated facilitating ease of positioning. The source operates with a few nJ per laser pulse, making this a versatile emitter that enables nanometrology, multisource electron-lithography and scanning probe microscopy.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Strong-field ionization of plasmonic nanoparticles

We modeled strong-field ionization of metal nanoparticles by intense infrared laser pulses, accounting for and distinguishing in photoelectron (PE) momentum distributions the effects of PE correlation, PE–residual-charge interactions, PE rescattering and recombination, and transient laser-induced plasmonic fields. Our numerical results for 5-, 30-, and 70-nm-diameter gold nanospheres and peak laser-pulse intensities of 8.0×10 12 and 1.2×10 13 W/cm 2 show how PE velocity-map images are distinctly shaped by PE Coulomb repulsion, residual-charge accumulations, and plasmonic near fields. In contrast to gaseous atomic targets and dielectric nanoparticles, we find very large PE cutoff energies, for both directly emitted and rescattered PEs, that exceed the incident laser-pulse ponderomotive energy by two orders of magnitude.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2023

Thermal transfer enhancement by hydrodynamic plasmons in electron bilayers

Here, we develop a theory of heat transfer induced by thermal charge fluctuations in two-dimensional electron double layers. We consider pristine systems comprised of identical layers and focus on the regime of sufficiently high temperatures and interlayer distances 𝑑, where the relevant charge fluctuations may be described using the hydrodynamic approach. In this limit heat transfer is dominated by the plasmon resonances. For systems with Galilean-invariant electron dispersion the interlayer thermal conductance 𝜘 is proportional to the kinematic viscosity of the electron liquid and decreases as 1/𝑑 4 . In the absence of Galilean invariance 𝜘∝𝜎/𝑑 3 , where 𝜎 is the intrinsic conductivity of the liquid. This strong enhancement can be traced to a drastically different broadening of plasmon resonances in systems with and without Galilean invariance.

2-dimensional systems↗

DOE OSTI2019

Nonlinear Plasmonic Photoelectron Response of Ag(111)

Photons can excite collective and single-particle excitations in metals; the collective plasmonic excitations are of keen interest in physics, chemistry, optics, and nanotechnology because they enhance coupling of electromagnetic energy and can drive nonlinear processes in electronic materials, particularly where their dielectric function ϵ(ω) approaches zero. Here, we investigate the nonlinear angle-resolved two-photon photoemission (2PP) spectroscopy of the Ag(111) surface through the ϵ(ω) near-zero region. In addition to the Einsteinian single-particle photoemission, the 2PP spectra report unequivocal signatures of nonlocal dielectric, plasmonically enhanced, excitation processes.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2016

Near-Field Spectroscopy and Imaging of Subwavelength Plasmonic Terahertz Resonators

We describe the temporal evolution of the terahertz (THz) field leading to the excitation of plasmonic resonances in carbon microfibers. The field evolution is mapped in space and time for the 3/2 wavelength resonance using a subwavelength aperture THz near-field probe with an embedded THz photoconductive detector. The excitation of surface waves at the fiber tips leads to the formation of a standing wave along the fiber. Local THz time-domain spectroscopy at one of the standing wave crests shows a clear third-order resonance peak at 1.65 THz, well described by the Lorentz model. Lastly, this application of the subwavelength aperture THz near-field microscopy for mode mapping and local spectroscopy demonstrates the potential of near-field methods for studies of subwavelength plasmonic THz resonators.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗