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Nanoimprint Lithography Facilitated Plasmonic-Photonic Coupling for Enhanced Photoconductivity and Photocatalysis
Imprint lithography has emerged as a reliable, reproducible, and rapid method for patterning colloidal nanostructures. As a promising alternative to top-down lithographic approaches, the fabrication of nanodevices has thus become effective and straightforward. In this study, a fusion of interference lithography (IL) and nanosphere imprint lithography on various target substrates ranging from carbon film on transmission electron microscope grid to inorganic and dopable polymer semiconductor is reported. 1D plasmonic photonic crystals are printed with 75% yield on the centimeter scale using colloidal ink and an IL-produced polydimethylsiloxane stamp. Atomically smooth facet, single-crystalline, and monodisperse colloidal building blocks of gold (Au) nanoparticles are used to print 1D plasmonic grating on top of a titanium dioxide (TiO2) slab waveguide, producing waveguide-plasmon polariton modes with superior 10 nm spectral line-width. Plasmon-induced hot electrons are confirmed via two-terminal current measurements with increased photoresponsivity under guiding conditions. The fabricated hybrid structure with Au/TiO2 heterojunction enhances photocatalytic processes like degradation of methyl orange (MO) dye molecules using the generated hot electrons. This simple colloidal printing technique demonstrated on silicon, glass, Au film, and naphthalenediimide polymer thus marks an important milestone for large-scale implementation in optoelectronic devices. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
Direct Observation of Plasmon Band Formation and Delocalization in Quasi-Infinite Nanoparticle Chains
Chains of metallic nanoparticles sustain strongly confined surface plasmons with relatively low dielectric losses. To exploit these properties in applications, such as waveguides, the fabrication of long chains of low disorder and a thorough understanding of the plasmon-mode properties, such as dispersion relations, are indispensable. Here, we use a wrinkled template for directed self-assembly to assemble chains of gold nanoparticles. With this up-scalable method, chain lengths from two particles (140 nm) to 20 particles (1500 nm) and beyond can be fabricated. Electron energy-loss spectroscopy supported by boundary element simulations, finite-difference time-domain, and a simplified dipole coupling model reveal the evolution of a band of plasmonic waveguide modes from degenerated single-particle modes in detail. In striking difference from plasmonic rod-like structures, the plasmon band is confined in excitation energy, which allows light manipulations below the diffraction limit. The non-degenerated surface plasmon modes show suppressed radiative losses for efficient energy propagation over a distance of 1500 nm. © 2019 American Chemical Society.
Exploiting Combinatorics to Investigate Plasmonic Properties in Heterogeneous Ag-Au Nanosphere Chain Assemblies
Chains of coupled metallic nanoparticles are of special interest for plasmonic applications because they can sustain highly dispersive plasmon bands, allowing strong ballistic plasmon wave transport. Whereas early studies focused on homogeneous particle chains exhibiting only one dominant band, heterogeneous assemblies consisting of different nanoparticle species came into the spotlight recently. Their increased configuration space principally allows engineering multiple bands, bandgaps, or topological states. Simultaneously, the challenge of the precise arrangement of nanoparticles, including their distances and geometric patterns, as well as the precise characterization of the plasmonics in these systems, persists. Here, the surface plasmon resonances in heterogeneous Ag-Au nanoparticle chains are reported. Wrinkled templates are used for directed self-assembly of monodisperse gold and silver nanospheres as chains, which allows assembling statistical combinations of more than 109 particles. To reveal the spatial and spectral distribution of the plasmonic response, state-of-the-art scanning transmission electron microscopy coupled with electron energy loss spectroscopy accompanied by boundary element simulations is used. A variety of modes in the heterogeneous chains are found, ranging from localized surface plasmon modes occurring in single gold or silver spheres, respectively, to modes that result from the hybridization of the single particles. This approach opens a novel avenue toward combinatorial studies of plasmonic properties in heterosystems. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
NaOH protective layer for a stable sodium metal anode in liquid electrolytes
Sodium is known as a soft metal that can easily change its particle morphology. It can form outstretched and rolled fibers with plastic or brittle behavior, and cubes. In Na-batteries, metallic Na anodes demonstrate a high reactivity towards the majority of electrolyte solutions, volume change and a random deposition process from the electrolyte, accompanied by dendrite formation. In order to smooth the electrochemical Na deposition, we propose NaOH as a simple artificial protective layer for sodium, formed by its exposure to ambient conditions for a certain period of time. The formed NaOH layer on top of the metallic sodium suppresses the volume change and dendrite growth on the sodium surface. Additionally, the protected sodium does not change its morphology after a prolonged contact with carbonate-based electrolytes. In symmetric Na-batteries, the NaOH layer increases the lifetime of the electrochemical cell by eight times in comparison to non-protected Na. In the full-cell with a layered sodium oxide cathode, the NaOH-protected sodium anode also leads to a high cycling stability, providing 81 % of the initial cell capacity after 500 cycles with a 1C current rate. In contrast, batteries with a non-protected Na-anode reach only 20 % of their initial capacity under the same conditions. Therefore, the main benefits of the NaOH artificial layer are the chemical compatibility with the carbonate-based electrolytes, the protection of Na metal against reaction with the electrolyte solution, the rapid Na-ion diffusion through the layer and the formation of a mechanical barrier, mitigating Na-dendrite growth. This work presents an easily scalable method to protect sodium without any additional chemicals or a special environment for this reaction.
Tailoring Plasmonics of Au@Ag Nanoparticles by Silica Encapsulation
Hybrid metallic nanoparticles (NPs) encapsulated in oxide shells are currently intensely studied for plasmonic applications in sensing, medicine, catalysis, and photovoltaics. Here, a method for the synthesis of Au@Ag@SiO2 cubes with a uniform silica shell of variable and adjustable thickness in the nanometer range is introduced and their excellent, highly reproducible, and tunable optical response is demonstrated. Varying the silica shell thickness, the excitation energies of the single NP plasmon modes can be tuned in a broad spectral range between 2.55 and 3.25 eV. Most importantly, a strong coherent coupling of the surface plasmons is revealed at the silver–silica interface with Mie resonances at the silica–vacuum interface leading to a significant field enhancement at the encapsulated NP surface in the range of 100% at shell thicknesses t ≃ 20 nm. Consequently, the synthesis method and the field enhancement open pathways to a widespread use of silver NPs in plasmonic applications including photonic crystals and may be transferred to other non-precious metals. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
Axion Mie theory of electron energy loss spectroscopy in topological insulators
Electronic topological states of matter exhibit novel types of responses to electromagnetic fields. The response of strong topological insulators, for instance, is characterized by a so-called axion term in the electromagnetic Lagrangian which is ultimately due to the presence of topological surface states. Here we develop the axion Mie theory for the electromagnetic response of spherical particles including arbitrary sources of fields, i.e., charge and current distributions. We derive an axion induced mixing of transverse magnetic and transverse electric modes which are experimentally detectable through small induced rotations of the field vectors. Our results extend upon previous analyses of the problem. Our main focus is on the experimentally relevant problem of electron energy loss spectroscopy in topological insulators, a technique that has so far not yet been used to detect the axion electromagnetic response in these materials.