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- ItemExploiting Combinatorics to Investigate Plasmonic Properties in Heterogeneous Ag-Au Nanosphere Chain Assemblies(Weinheim : Wiley-VCH, 2021) Schletz, Daniel; Schultz, Johannes; Potapov, Pavel L.; Steiner, Anja Maria; Krehl, Jonas; König, Tobias A.F.; Mayer, Martin; Lubk, Axel; Fery, AndreasChains 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
- ItemTailoring Plasmonics of Au@Ag Nanoparticles by Silica Encapsulation(Weinheim : Wiley-VCH, 2021) Schultz, Johannes; Kirner, Felizitas; Potapov, Pavel; Büchner, Bernd; Lubk, Axel; Sturm, Elena V.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
- ItemFreestanding Nanolayers of a Wide-Gap Topological Insulator through Liquid-Phase Exfoliation(Weinheim : Wiley-VCH, 2021) Lê Anh, Mai; Potapov, Pavel; Wolf, Daniel; Lubk, Axel; Glatz, Bernhard; Fery, Andreas; Doert, Thomas; Ruck, MichaelThe layered salt Bi14Rh3I9 is a weak three-dimensional (3D) topological insulator (TI), that is, a stack of two-dimensional (2D) TIs. It has a wide non-trivial band gap of 210 meV, which is generated by strong spin-orbit coupling, and possesses protected electronic edge-states. In the structure, charged layers of (Formula presented.) (Bi4Rh)3I]2+ honeycombs and (Formula presented.) Bi2I8]2− chains alternate. The non-trivial topology of Bi14Rh3I9 is an inherent property of the 2D intermetallic fragment. Here, the exfoliation of Bi14Rh3I9 was performed using two different chemical approaches: (a) through a reaction with n-butyllithium and poly(vinylpyrrolidone), (b) through a reaction with betaine in dimethylformamide at 55 °C. The former yielded few-layer sheets of the new compound Bi12Rh3I, while the latter led to crystalline sheets of Bi14Rh3I9 with a thickness down to 5 nm and edge-lengths up to several ten microns. X-ray diffraction and electron microscopy proved that the structure of Bi14Rh3I9 remained intact. Thus, it was assumed that the particles are still TIs. Dispersions of these flakes now allow for next steps towards the envisioned applications in nanoelectronics, such as the study of quantum coherence in deposited films, the combination with superconducting particles or films for the generation of Majorana fermions, or studies on their behavior under the influence of magnetic or electric fields or in contact with various materials occurring in devices. The method presented generally allows to exfoliate layers with high specific charges and thus the use of layered starting materials beyond van der Waals crystals. © 2020 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH