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At least 181 records · Page 10

Engineering Directionality in Quantum Dot Shell Lasing Using Plasmonic Lattices

In this paper, we report how the direction of quantum dot (QD) lasing can be engineered by exploiting high-symmetry points in plasmonic nanoparticle (NP) lattices. The nanolaser architecture consists of CdSe-CdS core-shell QD layers conformally coated on two-dimensional square arrays of Ag NPs. Using waveguide-surface lattice resonances (W-SLRs) near the Δ point in the Brillouin zone as optical feedback, we achieved lasing from the gain in CdS shells at off-normal emission angles. Changing the periodicity of the plasmonic lattices enables other high-symmetry points (Γ or M) of the lattice to overlap with the QD shell emission, which facilitates tuning of the lasing direction. We also increased the thickness of the QD layer to introduce higher order W-SLR modes with additional avoided crossings in the band structure, which expands the selection of cavity modes for any desired lasing emission angle.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Active Temporal Control of Radiative Heat Transfer with Graphene Nanodisks

The ability to dynamically control the radiative transfer of heat at the nanoscale holds the key to the development of a diverse number of technologies, ranging from nanoscale thermal-management systems to improved thermophotovoltaic devices. Recently, graphene has emerged as an ideal material to achieve this goal, since it can be electrically doped to support surface plasmons, collective oscillations of the conduction electrons. These resonances produce large and spectrally narrow optical cross sections, which dictate the emission and absorption properties of the graphene nanostructure and, thus, the heat that it radiatively exchanges with other objects and the environment. For attainable levels of doping, the plasmons supported by graphene nanostructures naturally lie in the midinfrared part of the spectrum, which is the most relevant wavelength range for radiative heat transfer under realistic temperatures. Furthermore, these resonances are actively tunable, thus providing full dynamic control over the heat transfer. Motivated by this great potential, we present a comprehensive analysis of the temporal evolution of the radiative heat transfer between arrangements of graphene nanodisks, showing that it is possible to exploit the tunability of these structures to obtain actively controlled heat transfer scenarios not possible with conventional passive nanostructures. We report the results of this work provide a framework for achieving fully dynamical control over nanoscale radiative heat transfer and thus provide fundamental insights into this process.

36 MATERIALS SCIENCE↗

Plasmonically assisted channels of photoemission from metals

We analyze recently measured nonlinear photoemission spectra from Ag surfaces that reveal resonances whose energies do not scale with the applied photon energy but stay pinned to multiples of bulk plasmon energy $\hbar$ω p above the Fermi level. To elucidate these unexpected and peculiar features we investigate the spectra of plasmons generated in a solid by the optically pumped electronic polarization and their effect on photoemission. By combining quadratic response formalism for calculations of photoemission yield, a nonperturbative approach to inelastic electron scattering, and first-principles calculations for the electronic structure, we demonstrate the dependence of probability amplitude for single- and multiplasmon excitations on the basic parameters characterizing the photon pulse and the system. The resulting multiexcitation spectrum evolves towards a truncated plasmonic coherent state. Analogous concept is extrapolated to interpret plasmon generation by multiphoton excited electronic polarization. Based on this we elaborate a scenario that the thus created real plasmons act as supplementary frequency-locked pump field for non-Einsteinian plasmonically assisted channels of photoemission from metals. The established paradigm enables assignment and assessment of the observed linear $\hbar$ω p and nonlinear 2$\hbar$ω p electron yields from Ag. Such effects may be exploited for selective filtering of optical energy conversion in electronic systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Surface Josephson plasma waves in a high-temperature superconductor

Abstract Electron density oscillations with acoustic dispersions and sustained at boundaries between different media provide information about surface and interface properties of heterostructures. In ultrathin metallic films these plasmonic excitations are heavily damped. Superconductivity is predicted to reduce dissipation allowing detection of these resonances. Emerging low-loss interface Cooper-pair waves have been studied before, however, the observation of surface-confined Josephson plasmons in highly anisotropic superconductors has remained elusive. Here, we report on generation and coupling to these excitations in an ultrathin single-crystal film of high-temperature superconductor La 1.85 Sr 0.15 CuO 4 . The film becomes brighter than Au below the critical temperature when probed with sub-gap THz photons. We show that the enhanced signal in the superconducting state, which can be visualized with a spatial resolution better than λ/3000, originates from near-field coupling of light to surface Josephson plasmons. Our results open a path towards non-invasive investigation of enhanced superconductivity in artificial multilayers, buried interface states in topological heterostructures, and non-linear phenomena in Josephson devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Broadband Asymmetric Transmission of Linearly Polarized Mid‐Infrared Light Based on Quasi‐3D Metamaterials

Abstract Metamaterials consisting of subwavelength resonators offer an exciting opportunity for realizing asymmetric transmission (AT) of linearly polarized light. However, to date, only moderate/narrow‐band AT responses have been obtained in metadevices based on stacked planar nanostructures. Here, leveraging a combination of a genetic algorithm (GA) based optimization method and a membrane projection lithography (MPL) fabrication approach, a quasi‐3D metamaterial for broadband AT of linearly polarized mid‐infrared light is demonstrated. Facilitated by the customized GA, an efficient exploration of 3D plasmonic meta‐atoms with broken mirror symmetry in the light propagation direction allows the satisfaction of the rigorous conditions for AT of linearly polarized waves over a broad wavelength range. Confirmed by surface current analysis, the observed AT behavior is attributed to the resonant coupling between the plasmonic nanostructures located on the two orthogonal walls of the MPL cavities. Incorporating an advanced inverse‐design method and a state‐of‐art fabrication technique, the methodology used in the present study provides a promising route for exploiting 3D metamaterials with sophisticated functionalities via effectively exploring the high‐dimensional parametric space offered by true 3D meta‐atoms.

Whiting, Eric B.↗

Retarded Charge-Carrier Recombination in Photoelectrochemical Cells from Plasmon-Induced Resonance Energy Transfer

N-type metal oxides such as hematite (α-Fe 2 O 3 ) and bismuth vanadate (BiVO 4 ) are promising candidate materials for efficient photoelectrochemical water splitting; however, their short minority carrier diffusion length and restricted carrier lifetime result in undesired rapid charge recombination. In this paper, a 2D arranged globular Au nanosphere (NS) monolayer array with a highly ordered hexagonal hole pattern (hereafter, Au array) is introduced onto the surface of photoanodes comprised of metal oxide films via a facile drying and transfer-printing process. Through plasmon-induced resonance energy transfer, the Au array provides a strong electromagnetic field in the near-surface area of the metal oxide film. The near-field coupling interaction and amplification of the electromagnetic field suppress the charge recombination with long-lived photogenerated holes and simultaneously enhance the light harvesting and charge transfer efficiencies. Consequently, an over 3.3-fold higher photocurrent density at 1.23 V versus reversible hydrogen electrode (RHE) is achieved for the Au array/α-Fe 2 O 3 . Furthermore, the high versatility of this transfer printing of Au arrays is demonstrated by introducing it on the molybdenum-doped BiVO 4 film, resulting in 1.5-fold higher photocurrent density at 1.23 V versus RHE. The tailored metal film design can provide a potential strategy for the versatile application in various light-mediated energy conversion and optoelectronic devices.

2D pattern array↗

High-Quality Surface Plasmon Polaritons in Large-Area Sodium Nanostructures

Sodium (Na) is predicted to be an ideal plasmonic material with ultralow optical loss across visible to near-infrared (NIR). However, there has been limited research on Na plasmonics. We develop a scalable fabrication method for Na nanostructures by combining phase-shift photolithography and a thermo-assisted spin-coating process. Using this method, we fabricated Na nanopit arrays with varying periodicities (300-600 nm) and with tunable surface plasmon polariton (SPP) modes spanning visible to NIR. We achieved SPP resonances as narrow as 9.3 nm. In addition, Na nanostructures showed line width narrowing from visible toward NIR, showing their prospect operating in the NIR. To address the challenges associated with the high reactivity of Na, we designed a simple encapsulation strategy and stabilized the Na nanostructures in ambient conditions for more than two months. As a low-cost and low-loss plasmonic material, Na offers a competitive option for nanophotonic devices and plasmon-enhanced applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

An Overview of Nanomaterials for Environmental Remediation Applications

The environmental remediation capabilities of nanoparticles were reviewed and evaluated. Nanoparticles (NPs) have been used to remediate various forms of environmental contamination. Various materials, morphologies, and conditions are required to remediate different contaminants. Nanoparticles may have benefits and/or limitations compared with traditional remediation methods. New techniques are being applied to mitigate the limitations of NPs. Nanomaterials are a promising technology for the environmental remediation. NPs have been used for the remediation of aqueous and atmospheric contaminants. Nanoparticles have been used to sequester contaminants toxic to human and environmental health. Various materials, morphologies, and conditions are necessary for the remediation of different contaminants. The remediation of heavy metals is of significant concern. Contaminants may be remediated by means of sorption or reduction. The remediation capability of nanoparticles is promising due to their high surface area and reactivity. Reaction kinetics are, therefore, notably fast. These characteristics make NPs attractive for environmental remediation. Various NPs have been used as sequestering agents for environmental contaminants. NPs have been used to remediate heavy metals as well as organic contaminants. Technical Objectives: Assess viability of nanoparticles (NPs) for environmental remediation; Review benefits and limitations of NPs; Design future experiments to test remediation capabilities of NPs. Future Plans: Create NP filters for remediation - Grow Au NPs on Stainless Steel Wool: Stainless steel wool has many defects and crevices allowing the Au NPs to grow on the surface; Stainless steel wool will not react with the heavy metal contaminants tested; NPs are embedded, so they do not have to be removed from solution. Test sorption capabilities with heavy metal contaminants in aqueous solution. Benefits of Gold NPs: Corrosion/oxidation resistant; Exhibit visible/near IR plasmon resonance; Can be synthesized by solution chemistry: cost efficient and easily scalable. Surfactants: Used to lower surface energy and prevent aggregation; Sodium citrate: anionic surfactant (-); Cetyltrimethylammonium bromide (CTAB): cationic surfactant (+); Ionic surfactants create charged NPs; Charged NPs can be used to sequester ionic contaminants (eg. heavy metals)

54 ENVIRONMENTAL SCIENCES↗

High power edge-cum-surface emitting terahertz laser arrays phased locked by vacuum guided plasmon waves

Terahertz semiconductor quantum-cascade lasers (QCLs) are widely implemented with metallic cavities that support low-loss plasmonic optical modes at long wavelengths. However, resonant optical modes in such cavities suffer from poor radiative characteristics due to their subwavelength transverse dimensions. Consequently, single-mode terahertz QCLs with metallic cavities and large (>100 mW) output power have only been realized in the surface-emitting configuration that affords a large radiating surface. Here, we demonstrate a method to enhance radiative outcoupling from such plasmonic lasers for high-power emission in the edge-emitting (end-fire or longitudinal) direction. Single-sided plasmon waves propagating in vacuum are resonantly excited in surrounding medium of metallic cavities with the QCL semiconductor medium. The vacuum guided plasmon waves with a large wavefront phase-lock multiple metallic cavities longitudinally, which leads to intense radiation in multiple directions, including that in the longitudinal direction in a narrow single-lobed beam. The multicavity array radiates predominantly in a single spectral mode. A peak-power output of 260 mW and a slope efficiency of 303 mW/A are measured for the end-fire beam from a 3.3 THz QCL operating at 54 K in a Stirling cooler. Finally, single-mode operation and lithographic tuning across a bandwidth of ~150 GHz are demonstrated.

42 ENGINEERING↗

Lasing from Finite Plasmonic Nanoparticle Lattices

Small lasers can generate coherent light for integrated photonics, in-vivo cellular imaging, and solid-state lighting. Unlike conventional lasers, plasmonic lasers can generate coherent light at sub-wavelength scales, although cavity architectures based on metal films and semiconducting gain exhibit large radiative losses and lack directional emission. In contrast, two-dimensional (2D) metal nanoparticle arrays surrounded by organic dyes can support lasing with high directionality at room temperature. Yet, the relationship between the number of nanoparticles in a finite lattice and their lasing emission characteristics is unknown. Here we show that the number of units in 2D gold nanoparticle lattices is critical to generate robust cavity resonances and lasing emission. Narrower lattice plasmons associated with stronger electromagnetic near fields are observed as nanoparticle number increases. Experimentally, we demonstrate lasing from a 30x30 nanoparticle lattice. Semi-quantum modeling indicates lower lasing thresholds and faster population inversion dynamics with higher nanoparticle numbers. These findings indicate that finite lattices of nanoparticles integrated with gain can function as independent, coherent light sources for optical multiplexing and lab-on-a-chip applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Experimental Demonstration of Dark‐State Metasurface Laser with Controllable Radiative Coupling

Abstract Lasing at the nanoscale using plasmonic nanoparticles offers the prospect of strong field concentration, hence strong light−matter interactions, low lasing thresholds, and ultrafast operation. However plasmonic nanoparticles suffer from high dissipative and radiative losses, the latter being rigidly tied to the shape of the nanoparticles and symmetry of their localized plasmon resonant modes. To overcome this limitation, recent theoretical work proposes using direct lasing into dark surface states to construct lasers that conceptually allow for independent implementation of the lasing state and its coherent radiation output. Here, lasing in dark resonant states of a metasurface laser and controllable coherent outcoupling of radiation with the aid of a tightly coupled, weakly radiative metasurface are demonstrated experimentally. The laser is implemented using a thin, low‐loss dielectric film supporting surface mode‐like dark dielectric bound states and the coupling metasurface is composed of small non‐resonant scatterers that controllably but weakly perturb the dark mode and turn it partially bright. Distinct far‐field signatures that can be observed experimentally for both dark and bright lasing are identified and demonstrated. The scalability of this design, here implemented for lasing in the near‐infrared, enables large‐aperture ultra‐thin coherent light sources with controllable emission from the infrared to the visible.

36 MATERIALS SCIENCE↗

Micrometer-accuracy 2D displacement interferometer with plasmonic metasurface resonators

In this Letter, a high-accuracy, two-dimensional displacement sensor is proposed, designed, and demonstrated based on the concept of an extrinsic Fabry–Perot Interferometer. The sensor is composed of two bundled single-mode optic fibers in parallel and two plasmonic metasurface resonators inscribed on a gold substrate via a focused ion beam. The fiber end surface and the metasurface are in parallel with a small cavity between. The cavity change or Z -component displacement is determined from the pattern of interference fringes. The X -component displacement, perpendicular to the Z component, is identified from wavelength-selective metasurface resonators, which possess unique resonant wavelengths due to different nanostructure designs. The sensor was calibrated with six displacements applied through a three-axis precision linear stage. Test results indicated that the proposed interferometer can measure displacements with a maximum error of 5.4 µm or 2.2%.

Guo, Chuanrui (ORCID:0000000271412972)↗

Active Plasmonics and Active Chiral Plasmonics through Orientation-Dependent Multipolar Interactions

While most active plasmonic efforts focus on responsive metamaterials to modulate optical response, we present a simple alternative based on applied orientation control that can likely be implemented for many passive plasmonic materials. Passive plasmonic motifs are simpler to prepare but cannot be altered postfabrication. Here, we show that such systems can be easily manipulated through substrate orientation control to generate both active plasmonic and active chiral plasmonic responses. Using gold nanocrescents as our model platform, we demonstrate tuning of optical extinction from -21% to +36% at oblique incidence relative to normal incidence. Variation of substrate orientation in relation to incident polarization is also demonstrated to controllably switch chiroptical handedness (e.g., Δg = ± 0.55). These active plasmonic responses arise from the multipolar character of resonant modes. In particular, we correlate magnetoelectric and dipole–quadrupole polarizabilities with different light-matter orientation-dependence in both near- and far-field localized surface plasmon activity. Additionally, the attribution of far-field optical response to higher-order multipoles highlights the sensitivity offered by these orientation-dependent characterization techniques to probe the influence of localized electromagnetic field gradients on a plasmonic response. The sensitivity afforded by orientation-dependent optical characterization is further observed by the manifestation in both plasmon and chiral plasmon responses of unpredicted structural nanocrescent variance (e.g., left- and right-tip asymmetry) not physically resolved through topographical imaging.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanoscale Imaging of Optical-Frequency Plasmonic Energy Transfer in Individual Nanoparticles and their Assemblies

The nonradiative transfer of energy from plasmonic metal nanostructures to their neighboring environments is a rapidly expanding research area because of its tremendous potential impact on photovoltaics and photocatalysis. Despite the significant progress achieved via optical spectroscopies, understanding the differing and competing energy transfer pathways available to these systems still presents a major challenge due to a lack of insight into their nanoscale optical responses. With the atom-scale spatial resolving power of the electron microscope and its ability to probe optical transitions, electron spectroscopies like EELS are uniquely suited for these challenges. Our proposal addressed STEM/EELS techniques (Camden) to directly measure and even control energy transfer pathways in hybrid plasmon-resonator systems and leveraged detailed theoretical models combined with simulation (Masiello) to understand the essential underlying physics. In particular, the outcome of our proposed studies deepened the fundamental understanding of how surface plasmons shed energy to their environment and the practical knowledge gained here will influence the design of future high-efficiency solar energy-harvesting devices and photocatalysts capable of operating throughout the visible and the infrared.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Identification of Brillouin Zones by In-Plane Lasing from Light-Cone Surface Lattice Resonances

Periodic optical structures can control the flow of light, which has facilitated applications in optical fibers, laser cavities, and biochemical sensors. The first Brillouin zone (BZ) in reciprocal space can describe all the electromagnetic fields localized inside a photonic lattice. However, photonic lattices also exhibit radiative losses from light scattering, but the radiated fields are not captured by the first BZ. In a two-dimensional lattice, the in-plane wavevectors of photonic modes are limited by the so-called light cone, which depicts free-photon dispersion relations in the surrounding medium. Here we show that projection of the light cone on extended BZs provides a geometric method to observe radiated electromagnetic fields of photonic lattice modes. We developed a coupled dipole radiation theory to reveal how lattice geometry and dipole orientation affect the angular distributions of the radiated fields. Using dye molecules as local dipole emitters to excite and probe the optical modes, we experimentally identified high-order BZ edges through directional, in-plane lasing emission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Phonon modulation of strongly coupled gold tetrahedral plasmonic nanoparticles and a carbocyanine J-aggregate

Coupling exciton and plasmon excitations to form polaritons are of great interest for manipulating energy transfer at the nanoscale via the formation of hybrid light–matter states. In this study, we successfully couple gold tetrahedral nanoparticles with the J-aggregate forming dye 5,5′,6,6′-tetrachloro-1,1′-diethyl-3,3′-di(4-sulfobutyl)-benzimidazolocarbocyanine (TDBC) to form a strongly coupled colloidal polariton system with a Rabi splitting energy of ∼206 meV. These gold tetrahedra exhibit coherent phonon modes upon photoexcitation, which produce transient oscillations of the LSPR energy for isolated tetrahedra. Transient absorption measurements of the polariton system were performed and show how these coherent phonon modes influence the polariton states’ extinction. We found that the oscillation period increases by 0.5 ± 0.14 ps upon surface deposition of TDBC dye, demonstrating LSPR sensitivity to the refractive index environment. Shifts in the plasmon resonance due to the coherent phonon modes transiently alters LSPR alignment with the J-aggregate exciton peak, resulting in shifts of the hybrid polariton states’ oscillator strength.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A Closer Look at Corrugated Au Tips

A series of optical and electron microscopies are utilized in concert to unravel the structural, optical, and plasmonic properties of corrugated metallic tips. While the overall microscopic shapes of the tips dictate their optical resonances and plasmonic field enhancement factors, nanometric structural details govern their tip-enhanced Raman (TER) spectra and images. Using 4-thiobenzonitrile (TBN) as a molecular reporter, spatially resolved TER spectra reveal that optical rectification and molecular charging are among the prominent observables in the tip-tip TER geometry. The comparisons we provide reinforce the complexity of what otherwise may be regarded as sharp tip probes. We show the spurious appearance of anions is driven by highly localized resonances that appear as a result of surface corrugation and their manifestation throughout the course of TER nano-spectroscopy complicates spectral assignments, particularly in works aimed at understanding plasmon-enhanced/induced chemical transformations through enhanced Raman spectroscopy and imaging. Overall, nanoscale spatial variations in the TERS spectra suggest that the tip-tip geometry sustains junction plasmons that appear very different from what may be expected from the hybridization of the bulk tip resonances.

Bhattarai, Ashish↗

Surface-Enhanced Raman Scattering Using Silica Whispering-Gallery Mode Resonators

The motivation of this work was to have robust spectroscopic sensors for sensitive detection and chemical analysis of organic and molecular compounds. The solution is to use silica sphere optical resonators to provide surface-enhanced spectroscopic signal. Whispering-gallery mode (WGM) resonators made from silica microspheres were used for surface-enhanced Raman scattering (SERS) without coupling to a plasmonic mechanism. Large Raman signal enhancement is observed by exclusively using 5.08-micron silica spheres with 785-nm laser excitation. The advantage of this non-plasmonic approach is that the active substrate is chemically inert silica, thermally stable, and relatively simple to fabricate. The Raman signal enhancement is broadly applicable to a wide range of molecular functional groups including aliphatic hydrocarbons, siloxanes, and esters. Applications include trace organic analysis, particularly for in situ planetary instruments that require robust sensors with consistent response.

Anderson, Mark S.↗