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- ItemProspects of Coupled Organic-Inorganic Nanostructures for Charge and Energy Transfer Applications(Weinheim : Wiley-VCH, 2021) Steiner, Anja Maria; Lissel, Franziska; Fery, Andreas; Lauth, Jannika; Scheele, MarcusWe review the field of organic–inorganic nanocomposites with a focus on materials that exhibit a significant degree of electronic coupling across the hybrid interface. These nanocomposites undergo a variety of charge and energy transfer processes, enabling optoelectronic applications in devices which exploit singlet fission, triplet energy harvesting, photon upconversion or hot charge carrier transfer. We discuss the physical chemistry of the most common organic and inorganic components. Based on those we derive synthesis and assembly strategies and design criteria on material and device level with a focus on photovoltaics, spin memories or optical upconverters. We conclude that future research in the field should be directed towards an improved understanding of the binding motif and molecular orientation at the hybrid interface. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemPlasmonic Properties of Colloidal Assemblies(Weinheim : Wiley-VCH, 2021) Rossner, Christian; König, Tobias A.F.; Fery, AndreasThe assembly of metal nanoparticles into supracolloidal structures unlocks optical features, which can go beyond synergistic combinations of the properties of their primary building units. This is due to inter-particle plasmonic coupling effects, which give rise to emergent properties. The motivation for this progress report is twofold: First, it is described how simulation approaches can be used to predict and understand the optical properties of supracolloidal metal clusters. These simulations may form the basis for the rational design of plasmonic assembly architectures, based on the desired functional cluster properties, and they may also spark novel material designs. Second, selected scalable state-of-the-art preparative strategies based on synthetic polymers to guide the supracolloidal assembly are discussed. These routes also allow for equipping the assembly structures with adaptive properties, which in turn enables (inter-)active control over the cluster optical properties. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
- ItemNanoimprint Lithography Facilitated Plasmonic-Photonic Coupling for Enhanced Photoconductivity and Photocatalysis(Weinheim : Wiley-VCH, 2021) Gupta, Vaibhav; Sarkar, Swagato; Aftenieva, Olha; Tsuda, Takuya; Kumar, Labeesh; Schletz, Daniel; Schultz, Johannes; Kiriy, Anton; Fery, Andreas; Vogel, Nicolas; König, Tobias A.F.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
- 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
- ItemConstrained thermoresponsive polymers - new insights into fundamentals and applications(Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2021) Flemming, Patricia; Münch, Alexander S.; Fery, Andreas; Uhlmann, PetraIn the last decades, numerous stimuli-responsive polymers have been developed and investigated regarding their switching properties. In particular, thermoresponsive polymers, which form a miscibility gap with the ambient solvent with a lower or upper critical demixing point depending on the temperature, have been intensively studied in solution. For the application of such polymers in novel sensors, drug delivery systems or as multifunctional coatings, they typically have to be transferred into specific arrangements, such as micelles, polymer films or grafted nanoparticles. However, it turns out that the thermodynamic concept for the phase transition of free polymer chains fails, when thermoresponsive polymers are assembled into such sterically confined architectures. Whereas many published studies focus on synthetic aspects as well as individual applications of thermoresponsive polymers, the underlying structure-property relationships governing the thermoresponse of sterically constrained assemblies, are still poorly understood. Furthermore, the clear majority of publications deals with polymers that exhibit a lower critical solution temperature (LCST) behavior, with PNIPAAM as their main representative. In contrast, for polymer arrangements with an upper critical solution temperature (UCST), there is only limited knowledge about preparation, application and precise physical understanding of the phase transition. This review article provides an overview about the current knowledge of thermoresponsive polymers with limited mobility focusing on UCST behavior and the possibilities for influencing their thermoresponsive switching characteristics. It comprises star polymers, micelles as well as polymer chains grafted to flat substrates and particulate inorganic surfaces. The elaboration of the physicochemical interplay between the architecture of the polymer assembly and the resulting thermoresponsive switching behavior will be in the foreground of this consideration.
- 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
- ItemStretchable Thin Film Mechanical-Strain-Gated Switches and Logic Gate Functions Based on a Soft Tunneling Barrier(Weinheim : Wiley-VCH, 2021) Chae, Soosang; Choi, Won Jin; Fotev, Ivan; Bittrich, Eva; Uhlmann, Petra; Schubert, Mathias; Makarov, Denys; Wagner, Jens; Pashkin, Alexej; Fery, AndreasMechanical-strain-gated switches are cornerstone components of material-embedded circuits that perform logic operations without using conventional electronics. This technology requires a single material system to exhibit three distinct functionalities: strain-invariant conductivity and an increase or decrease of conductivity upon mechanical deformation. Herein, mechanical-strain-gated electric switches based on a thin-film architecture that features an insulator-to-conductor transition when mechanically stretched are demonstrated. The conductivity changes by nine orders of magnitude over a wide range of tunable working strains (as high as 130%). The approach relies on a nanometer-scale sandwiched bilayer Au thin film with an ultrathin poly(dimethylsiloxane) elastomeric barrier layer; applied strain alters the electron tunneling currents through the barrier. Mechanical-force-controlled electric logic circuits are achieved by realizing strain-controlled basic (AND and OR) and universal (NAND and NOR) logic gates in a single system. The proposed material system can be used to fabricate material-embedded logics of arbitrary complexity for a wide range of applications including soft robotics, wearable/implantable electronics, human-machine interfaces, and Internet of Things.
- ItemControlling line defects in wrinkling: a pathway towards hierarchical wrinkling structures(London : Royal Soc. of Chemistry, 2021) Knapp, André; Nebel, Lisa Julia; Nitschke, Mirko; Sander, Oliver; Fery, AndreasWe demonstrate a novel approach for controlling the line defect formation in microscopic wrinkling structures by patterned plasma treatment of elastomeric surfaces. Wrinkles were formed on polydimethylsiloxane (PDMS) surfaces exposed to low-pressure plasma under uniaxial stretching and subsequent relaxation. The wrinkling wavelength λ can be regulated via the treatment time and choice of plasma process gases (H2, N2). Sequential masking allows for changing these parameters on micron-scale dimensions. Thus, abrupt changes of the wrinkling wavelength become feasible and result in line defects located at the boundary zone between areas of different wavelengths. Wavelengths, morphology, and mechanical properties of the respective areas are investigated by Atomic Force Microscopy and agree quantitatively with predictions of analytical models for wrinkle formation. Notably, the approach allows for the first time the realization of a dramatic wavelength change up to a factor of 7 to control the location of the branching zone. This allows structures with a fixed but also with a strictly alternating branching behavior. The morphology inside the branching zone is compared with finite element methods and shows semi-quantitative agreement. Thus our finding opens new perspectives for “programming” hierarchical wrinkling patterns with potential applications in optics, tribology, and biomimetic structuring of surfaces.