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At least 523 records · Page 29

Control of plasmons in topological insulators via local perturbations

Here, we use a fully quantum mechanical approach to demonstrate control of plasmonic excitations in prototype models of topological insulators by molecule-scale perturbations. Strongly localized surface plasmons are present in the host systems, arising from the topologically nontrivial single-particle edge states. A numerical evaluation of the random phase approximation equations for the perturbed systems reveals how the positions and the internal electronic structure of the added molecules affect the degeneracy of the locally confined collective excitations, i.e., shifting the plasmonic energies of the host system and changing their spatial charge density profile. In particular, we identify conditions under which significant charge transfer from the host system to the added molecules occurs. Furthermore, the induced field energy density in the perturbed topological systems due to external electric fields is determined.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Acoustic plasmons and conducting carriers in hole-doped cuprate superconductors

The layered crystal structures of cuprates enable collective charge excitations fundamentally different from those of three-dimensional metals. Acoustic plasmons have been observed in electron-doped cuprates by resonant inelastic X-ray scattering (RIXS); in contrast, whether acoustic plasmons exist in hole-doped cuprates is under debate, despite extensive measurements. This contrast led us to investigate the charge excitations of hole-doped cuprate La 2-x Sr x CuO 4 . Here we present incidentenergy-dependent RIXS measurements and calculations of collective charge response via the loss function to reconcile the aforementioned issues. Our results provide evidence for the acoustic plasmons of Zhang-Rice singlet (ZRS), which has a character of the Cu 3d x 2 -y 2 strongly hybridised with the O 2p orbitals; the metallic behaviour is implied to result from the movement of ZRS rather than the simple hopping of O 2p holes.

36 MATERIALS SCIENCE↗

Principles of two-dimensional terahertz spectroscopy of collective excitations: The case of Josephson plasmons in layered superconductors

Two-dimensional terahertz spectroscopy (2DTS), a terahertz analog of nuclear magnetic resonance, is a new technique poised to address many open questions in complex condensed matter systems. The conventional theoretical framework used ubiquitously for interpreting multidimensional spectra of discrete quantum level systems is, however, insufficient for the continua of collective excitations in strongly correlated materials. Here, in this work, we develop a theory for 2DTS of a model collective excitation, the Josephson plasma resonance in layered superconductors. Starting from a mean-field approach at temperatures well below the superconducting phase transition, we obtain expressions for the multidimensional nonlinear responses that are amenable to intuition derived from the conventional single-mode scenario. We then consider temperatures near the superconducting critical temperature T c , where dynamics beyond mean-field become important and conventional intuition fails. As fluctuations proliferate near T c , the dominant contribution to nonlinear response comes from an optical parametric drive of counterpropagating Josephson plasmons, which gives rise to 2D spectra that are qualitatively different from the mean-field predictions. As such, and in contrast to one-dimensional spectroscopy techniques, such as third harmonic generation, 2DTS can be used to directly probe thermally excited finite-momentum plasmons and their interactions. Our theory can readily be tested in cuprates, and we discuss implications beyond the present context of Josephson plasmons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dielectric function and plasmons in graphene: A self-consistent-field calculation within a Markovian master equation formalism

We introduce a method for calculating the dielectric function of nanostructures with an arbitrary band dispersion and Bloch wave functions. The linear response of a dissipative electronic system to an external electromagnetic field is calculated by a self-consistent-field approach within a Markovian master equation formalism (SCF-MMEF) coupled with full-wave electromagnetic equations. The SCF-MMEF accurately accounts for several concurrent scattering mechanisms. The method captures interband electron-hole-pair generation, as well as the interband and intraband electron scattering with phonons and impurities. We employ the SCF-MMEF to calculate the dielectric function, complex conductivity, and loss function for supported graphene. From the loss-function maximum, we obtain plasmon dispersion and propagation length for different substrate types [nonpolar diamondlike carbon (DLC) and polar SiO 2 and hBN], impurity densities, carrier densities, and temperatures. Plasmons on the two polar substrates are suppressed below the highest surface phonon energy, while the spectrum is broad on the nonpolar DLC. Plasmon propagation lengths are comparable on polar and nonpolar substrates and are on the order of tens of nanometers, considerably shorter than previously reported. As a result, they improve with fewer impurities, at lower temperatures, and at higher carrier densities.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Negative Refraction in Time-Varying Strongly Coupled Plasmonic-Antenna–Epsilon-Near-Zero Systems

Time-varying metasurfaces are emerging as a powerful instrument for the dynamical control of the electromagnetic properties of a propagating wave. Here we demonstrate an efficient time-varying metasurface based on plasmonic nano-antennas strongly coupled to an epsilon-near-zero (ENZ) deeply subwavelength film. The plasmonic resonance of the metal resonators strongly interacts with the optical ENZ modes, providing a Rabi level spitting of ~30%. Optical pumping at frequency ω induces a nonlinear polarization oscillating at 2ω responsible for an efficient generation of a phase conjugate and a negative refracted beam with a conversion efficiency that is more than 4 orders of magnitude greater compared to the bare ENZ film. In this work, the introduction of a strongly coupled plasmonic system therefore provides a simple and effective route towards the implementation of ENZ physics at the nanoscale.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Efficient Coupling and Transport of a Surface Plasmon at 780 nm in a Gold Nanostructure

We studied plasmonic nanostructures in single-crystal gold with scanning electron and femtosecond photoemission electron microscopies. We designed an integrated laser coupling and nanowire waveguide structure by focused ion beam lithography in single-crystal gold flakes. The photoemission results show that the laser field is efficiently coupled into a propagating surface plasmon by a simple hole structure and propagates efficiently in an adjacent nano-bar waveguide. A strong local field is created by the propagating surface plasmon at the nano-bar tip. A similar structure, with a decreased waveguide width and thickness, displayed significantly more intense photoemission indicating enhanced local electric field at the sharper tip.

Gong, Yu↗

Ultrafast nonlocal collective dynamics of Kane plasmon-polaritons in a narrow-gap semiconductor

The observation of ultrarelativistic fermions in condensed-matter systems has uncovered a cornucopia of novel phenomenology as well as a potential for effective ultrafast light engineering of new states of matter. While the nonequilibrium properties of two- and three-dimensional (2D and 3D) hexagonal crystals have been studied extensively, our understanding of the photoinduced dynamics in 3D single-valley ultrarelativistic materials is, unexpectedly, lacking. Here, we use ultrafast scanning near-field optical spectroscopy to access and control nonequilibrium large-momentum plasmon-polaritons in thin films of a prototypical narrow-bandgap semiconductor Hg 0.81 Cd 0.19 Te. We demonstrate that these collective excitations exhibit distinctly nonclassical scaling with electron density characteristic of the ultrarelativistic Kane regime and experience ultrafast initial relaxation followed by a long-lived highly coherent state. Our observation and ultrafast control of Kane plasmon-polaritons in a semiconducting material using light sources in the standard telecommunications fiber-optics window open a new avenue toward high-bandwidth coherent information processing in next-generation plasmonic circuits.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Infrared plasmons propagate through a hyperbolic nodal metal

Metals are canonical plasmonic media at infrared and optical wavelengths, allowing one to guide and manipulate light at the nanoscale. A special form of optical waveguiding is afforded by highly anisotropic crystals revealing the opposite signs of the dielectric functions along orthogonal directions. These media are classified as hyperbolic and include crystalline insulators, semiconductors, and artificial metamaterials. Layered anisotropic metals are also anticipated to support hyperbolic waveguiding. However, this behavior remains elusive, primarily because interband losses arrest the propagation of infrared modes. Here, we report on the observation of propagating hyperbolic waves in a prototypical layered nodal-line semimetal ZrSiSe. The observed waveguiding originates from polaritonic hybridization between near-infrared light and nodal-line plasmons. Unique nodal electronic structures simultaneously suppress interband loss and boost the plasmonic response, ultimately enabling the propagation of infrared modes through the bulk of the crystal.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Probing correlated states with plasmons

Understanding the nature of strongly correlated states in flat-band materials (such as moiré heterostructures) is at the forefront of both experimental and theoretical pursuits. While magnetotransport, scanning probe, and optical techniques are often very successful in investigating the properties of the underlying order, the exact nature of the ground state often remains unknown. Here, we propose to leverage strong light-matter coupling present in the flat-band systems to gain insight through dynamical dielectric response into the structure of the many-body ground state. We argue that because of the enlargement of the effective lattice of the system arising from correlations, conventional long-range plasmon becomes “folded” to yield a multiband plasmon spectrum. We detail several mechanisms through which the structure of the plasmon spectrum and that of the dynamical dielectric response is susceptible to the underlying order, revealing valued insights such as the interaction-driven band gaps, spin-structure, and the order periodicity.

36 MATERIALS SCIENCE↗

Driving energetically unfavorable dehydrogenation dynamics with plasmonics

Nanoparticle surface structure and geometry generally dictate where chemical transformations occur, with higher chemical activity at sites with lower activation energies. Here, we show how optical excitation of plasmons enables spatially modified phase transformations, activating otherwise energetically unfavorable sites. We have designed a crossed-bar Au-PdH x antenna-reactor system that localizes electromagnetic enhancement away from the innately reactive PdH x nanorod tips. Using optically coupled in situ environmental transmission electron microscopy, we track the dehydrogenation of individual antenna-reactor pairs with varying optical illumination intensity, wavelength, and hydrogen pressure. Our in situ experiments show that plasmons enable new catalytic sites, including dehydrogenation at the nanorod faces. Molecular dynamics simulations confirm that these new nucleation sites are energetically unfavorable in equilibrium and only accessible through tailored plasmonic excitation.

36 MATERIALS SCIENCE↗

Saturation of the two-plasmon parametric decay instability in experiments on the electron cyclotron plasma heating due to the extraordinary pump wave depletion

The saturation level of the low-threshold parametric two-plasmon instability of the extraordinary pump wave decay to two upper hybrid plasmons is analyzed under conditions when the only efficient saturation mechanism is the pump depletion. A closed system of differential equations describing both the instability excitation and saturation is derived. The system is solved numerically and an analytic expression is obtained for the anomalous absorption coefficient of the pump wave caused by the development of this instability. The saturation level of the two-plasmon decay instability and the related anomalous absorption efficiency are estimated from data obtained in experiments on the electron cyclotron resonance heating of the plasma by an extraordinary wave in the TEXTOR tokamak.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Designing graphene absorption in a multispectral plasmon-enhanced infrared detector

Here, we have examined graphene absorption in a range of graphene-based infrared devices that combine either monolayer or bilayer graphene with three different gate dielectrics. Electromagnetic simulations show that the optical absorption in graphene in these devices, an important factor in a functional graphene-based detector, is strongly dielectric-dependent. Our simulations reveal that plasmonic excitation in graphene can significantly influence the percentage of light absorbed in the entire device, as well as the graphene layer itself, with graphene absorption exceeding 25% in regions where plasmonic excitation occurs. Notably, the dielectric environment of graphene has a dramatic influence on the strength and wavelength range over which the plasmons can be excited, making dielectric choice paramount to final detector tunability and sensitivity.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Plasmon-phonon coupling between mid-infrared chiral metasurfaces and molecular vibrations

Plasmon-phonon coupling between metamaterials and molecular vibrations provides a new path for studying mid-infrared light-matter interactions and molecular detection. So far, the coupling between the plasmonic resonances of metamaterials and the phonon vibrational modes of molecules has been realized under linearly polarized light. Here, mid-infrared chiral plasmonic metasurfaces with high circular dichroism (CD) in absorption over 0.65 in the frequency range of 50 to 60 THz are demonstrated to strongly interact with the phonon vibrational resonance of polymethyl methacrylate (PMMA) molecules at 52 THz, under both left-handed and right-handed circularly polarized (LCP and RCP) light. The mode splitting features in the absorption spectra of the coupled metasurface-PMMA systems under both circular polarizations are studied in PMMA layers with different thicknesses. The relation between the mode splitting gap and the PMMA thickness is also revealed. The demonstrated results can be applied in areas of chiral molecular sensing, thermal emission, and thermal energy harvesting.

42 ENGINEERING↗

Tunability of indium tin oxide materials for mid-infrared plasmonics applications

Transparent conductive oxides (TCOs) have emerged as alternative plasmonic materials in recent years to replace noble metals. The advantages of TCOs include CMOS compatibility, tunability of optical and structural properties, and reduced losses. In this work, we demonstrate how post-deposition annealing of indium tin oxide (ITO) films in oxygen atmosphere allows for tuning their optical dispersion properties to the mid-infrared spectral range while simultaneously reducing their absorption losses. In particular, we show a materials strategy that extends the epsilon-near-zero (ENZ) point of ITO from the near-infrared to the mid-infrared range. This is demonstrated by fabricating periodic arrays of ITO discs of varying diameters and characterizing their plasmonic resonances in the mid-infrared range from λ = 5 to 10 µm. The developed ITO plasmonic structures pave the way to the development of novel infrared active devices for sensing and spectroscopy on a silicon-compatible platform.

36 MATERIALS SCIENCE↗

Ultrafast quantum photonics enabled by coupling plasmonic nanocavities to strongly radiative antennas

Quantum emitters coupled to plasmonic nanostructures can act as exceptionally bright sources of single photons, operating at room temperature. Plasmonic mode volumes supported by these nanostructures can be several orders of magnitude smaller than the cubic wavelength, which leads to dramatically enhanced light–matter interactions and drastically increased photon production rates. However, when increasing the light localization further, these deeply subwavelength modes may in turn hinder the fast outcoupling of photons into free space. Plasmonic hybrid nanostructures combining a highly confined cavity mode and a larger antenna mode circumvent this issue. We establish the fundamental limits for quantum emission enhancement in such systems and find that the best performance is achieved when the cavity and antenna modes differ significantly in size. We experimentally support this idea by photomodifying a nanopatch antenna deterministically assembled around a nanodiamond known to contain a single nitrogen–vacancy (NV) center. As a result, the cavity mode shrinks, further shortening the NV fluorescence lifetime and increasing the single-photon brightness. Our analytical and numerical simulation results provide intuitive insight into the operation of these emitter–cavity–antenna systems and show that this approach could lead to single-photon sources with emission rates up to hundreds of THz and efficiencies close to unity.

47 OTHER INSTRUMENTATION↗

Electrically tunable nonlinear light generation in plasmonic tunnel junctions

Active and efficient control of nonlinear optical processes is essential for integrated photonics, with applications in signal processing, ultrafast switching, and quantum light manipulation. While nanophotonic structures are powerful for enhancing nonlinearities, achieving wide-range electrical tunability has remained a challenge. Plasmonic tunnel junctions offer a unique path to bridge this gap because they combine extreme optical field confinement with direct electrical control in a single nanoscale device. Here, we report the first, to our knowledge, demonstration of electrically tunable second-harmonic generation (SHG) in plasmonic tunnel junctions. Using ultra-stable epitaxial heterostructures, we achieve reproducible modulation of SHG with depths up to ∼500% and magnitudes above 1.3V −1 . We identify two mechanisms, electric-field-induced SHG (EFISH) and ion migration, that can either compete or cooperate depending on junction thickness and bias, enabling both broad tunability and ferroelectric-like hysteretic switching. These findings establish plasmonic tunnel junctions as a platform for electrically controlled nonlinear optics, with potential for nanoscale light sources, reconfigurable modulators, and neuromorphic photonic devices..

42 ENGINEERING↗

Time Resolved Optical Studies on The Plasmonic Field Enhancement of Bacteriorhodopsin Proton Photo-current: Final Technical Report Covering Aug 31, 2015–Aug 31, 2016

Our research continues to focus on the effects of plasmonic nanoparticles on organic and inorganic light-harvesting materials. Recent work has focused on the synthesis of stabilized gold nanoparticles to enhance the efficiency of dye-sensitized solar cells (DSSCs). Two major concerns in dye sensitized solar cells (DSSCs) are efficient light absorption and charge collection. Charge collection typically suffers because transport of electrons through the mesoporous TiO 2 substrate is slow. Thus, one obvious way to improve charge collection is to reduce the thickness of the TiO 2 . Alternatively, a form of TiO 2 with fewer grain boundaries, such as nanotubes, could be used in place of sintered nanospheres. Unfortunately, both of these solutions end up reducing the amount of surface area available to adsorb dye molecules. This directly reduces the percentage of photons absorbed. This problem could be avoided if dye molecules with larger absorption were designed; although synthetic chemists seem to be pushing the limits of what is achievable. Plasmonic nanoparticles offer an alternative way to boost light absorption. It is well known that plasmonic nanoparticles can enhance the local electric field of resonant frequencies of light. If this were in the same spectral region as the dye’s absorption band it would increase the percentage of absorbed photons. One concern is that if the nanoparticles are too close to the dye molecules they can quench the excited state. To avoid this problem, we prepared gold nanoparticles with a silica shell. This limited the amount of quenching while still permitting some enhancement of absorption. Unfortunately, we ran into some serious issues. The iodide based electrolyte etched the gold nanoparticles, completely dissolving them within a few hours. The silica shell should have provided protection but there were pinholes through which iodide could diffuse. Increasing the thickness of the silica to over 10 nm prevented etching but also limited any photon absorption enhancement.

36 MATERIALS SCIENCE↗

Modeling and Fabrication of IR Photonic Devices for Plasmon-Mediated Catalysis and Sensor Applications

Sandia National Laboratories (SNL) and Southwest Research Institute (SWRI) collaborated on this CRADA to explore novel 3-D metamaterial structures or devices that are proficient at eliciting surface plasmon-polaritons at infrared (IR) frequencies. The derived structures play a central role in answering fundamental questions pertaining to the vibrational coupling of molecules with surface plasmons and the potential binding interactions or catalytic effects that result from this coupling. Three-D metamaterial samples fabricated at SNL were characterized by SWRI, showing potential utility for binding molecules with similar vibrational frequencies that match the plasmon-polaritons of the metamaterial structure.

36 MATERIALS SCIENCE↗