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- Item2D/3D Metallic Nano-objects Self-Organized in an Organic Molecular Thin Film(Washington, DC : ACS Publications, 2020) Molodtsova, Olga V.; Aristova, Irina M.; Potorochin, Dmitrii V.; Babenkov, Sergey V.; Khodos, Igor I.; Molodtsov, Serguei L.; Makarova, Anna A.; Smirnov, Dmitry A.; Aristov, Victor Yu.We present the fabrication and investigation of the properties of nanocomposite structures consisting of two-dimensional (2D) and three-dimensional (3D) metallic nano-objects self-organized on the surface and inside of organic molecular thin-film copper tetrafluorophthalocyanine (CuPcF4). Metallic atoms, deposited under ultrahigh vacuum (UHV) conditions onto the organic ultrathin film, diffuse along the surface and self-assemble into a system of 2D metallic overlayers. At the same time, the majority of the metal atoms diffuse into the organic matrix and self-organize into 3D nanoparticles (NPs) in a well-defined manner. The evolution of the morphology and electronic properties of such structures as a function of nominal metal content is studied under UHV conditions using transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HR-TEM), and photoelectron spectroscopy (PES) techniques. Using HR-TEM, we have observed the periodicity of atomic planes of individual silver NPs. The steady formation of agglomerates from individual single nanocrystallites with intercrystallite boundaries is observed as well. PES reveals generally weak chemical interactions between silver and the organic matrix and n-doping of CuPcF4 at the initial stages of silver deposition, which is associated with charge transfer from the 2D wetting layer on the basis of core-level spectra shift analysis. Copyright © 2020 American Chemical Society.
- ItemThe Anomalous Influence of Polyelectrolyte Concentration on the Deposition and Nanostructure of Poly(ethyleneimine)/Poly(acrylic acid) Multilayers(Basel : MDPI, 2019) Müller, MartinThe deposition and nanostructure of polyelectrolyte (PEL) multilayers (PEMs) of branched poly(ethyleneimine)/poly(acrylic acid) (PEI/PAA) onto silicon substrates was studied in terms of the dependence of pH and the PEL concentration (cPEL) in the individual adsorption steps z. Both a commercial automatic dipping device and a homebuilt automatic stream coating device (flow cell) were used. Gravimetry, SFM, transmission (TRANS) and in situ attenuated total reflection (ATR) FTIR spectroscopy were used for the quantitative determination of the adsorbed amount, thickness, chemical composition and morphology of deposited PEMs, respectively. Firstly, the combination of pH = 10 for PEI and pH = 4 for PAA, where both PEL were predominantly in the neutral state, resulted in an extraordinarily high PEM deposition, while pH combinations, where one PEL component was charged, resulted in a significantly lower PEM deposition. This was attributed to both PEL conformation effects and acid/base interactions between basic PEI and acidic PAA. Secondly, for that pH combination an exponential relationship between PEM thickness and adsorption step z was found. Thirdly, based on the results of three independent methods, the course of the deposited amount of a PEM-10 (z = 10) versus cPEL in the range 0.001 to 0.015 M at pH = 10/4 was non-monotonous showing a pronounced maximum at cPEL = 0.005 M. Analogously, for cPEL = 0.005 M a maximum of roughness and structure size was found. Fourthly, related to that finding, in situ ATR-FTIR measurements gave evidence for the release of outermost located PEI upon PAA immersion (even step) and of outermost PAA upon PEI immersion (odd step) under formation of PEL complexes in solution. These studies help us to prepare PEL-based films with a defined thickness and morphology for interaction with biofluids in the biomedical and food fields. © 2019 by the author.
- ItemAnomalous influence of salt concentration on deposition of poly(L-lysine)/cellulose sulfate multilayers evidenced by in situ ATR-FTIR(Basel : MDPI, 2020) Müller, MartinThe deposition of polyelectrolyte (PEL) multilayers (PEMs) of poly(L-lysine)/cellulose sulfate (PLL/CS) onto germanium (Ge) substrates depending on salt concentration (cS) and deposition step z at constant PEL concentration cPEL = 0.01 M and pH = 7.0 was studied. In situ ATR-FTIR spectroscopy was used for the quantitative determination of alternate PLL/CS deposition profiles (adsorbed amount versus z) and total deposited PEM amount. By varying cS from 0 M to 1.0 M, a maximum of deposited amount was obtained at 0.1 M, so that both no salinity (0 M) and high salinity (1.0 M) revealed deposited amounts that were far lower than for mean salinity (0.1 M). Furthermore, in situ ATR-FTIR allowed to determine the detailed modulation of the PEL composition during the consecutive PEM deposition, which was interpreted as being due to both diffusion of given PEL from the PEM interior towards the outermost region and release of the PEM upon contact with the bulk oppositely charged PEL solution. Finally, ex situ ATR-FTIR measurements on the PEL solutions after deposition of PEM-20 revealed the distinct release of PEL from the PEM solely for cS = 1.0 M, due to the highest mobility of PEL under high salt conditions. These studies help to prepare functional PEM coatings with defined thicknesses and morphologies for the passivation and activation of material surfaces in the biomedical and food field. © 2020 by the author.
- ItemPatterning and control of the nanostructure in plasma thin films with acoustic waves: mechanical vs. electrical polarization effects(Cambridge : RSC Publ., 2021) García-Valenzuela, Aurelio; Fakhfouri, Armaghan; Oliva-Ramírez, Manuel; Rico-Gavira, Victor; Rojas, Teresa Cristina; Alvarez, Rafael; Menzel, Siegfried B.; Palmero, Alberto; Winkler, Andreas; González-Elipe, Agustín R.Nanostructuration and 2D patterning of thin films are common strategies to fabricate biomimetic surfaces and components for microfluidic, microelectronic or photonic applications. This work presents the fundamentals of a surface nanotechnology procedure for laterally tailoring the nanostructure and crystalline structure of thin films that are plasma deposited onto acoustically excited piezoelectric substrates. Using magnetron sputtering as plasma technique and TiO2 as case example, it is demonstrated that the deposited films depict a sub-millimetre 2D pattern that, characterized by large lateral differences in nanostructure, density (up to 50%), thickness, and physical properties between porous and dense zones, reproduces the wave features distribution of the generated acoustic waves (AW). Simulation modelling of the AW propagation and deposition experiments carried out without plasma and under alternative experimental conditions reveal that patterning is not driven by the collision of ad-species with mechanically excited lattice atoms of the substrate, but emerges from their interaction with plasma sheath ions locally accelerated by the AW-induced electrical polarization field developed at the substrate surface and growing film. The possibilities of the AW activation as a general approach for the tailored control of nanostructure, pattern size, and properties of thin films are demonstrated through the systematic variation of deposition conditions and the adjustment of AW operating parameters.
- ItemLarge-area wet-chemical deposition of nanoporous tungstic silica coatings(London [u.a.] : RSC, 2015) Nielsen, K.H.; Wondraczek, K.; Schubert, U.S.; Wondraczek, L.We report on a facile procedure for synthesis of nanoporous coatings of tungstic silica through wet-chemical deposition and post-treatment of tungsten-doped potassium silicate solutions. The process relies on an aqueous washing and ion exchange step where dispersed potassium salt deposits are removed from a 150 nm silicate gel layer. Through an adjustment of the pH value of the washing agent within the solubility regime of a tungstic salt precursor, the tungsten content of the remaining nanostructured coating can be controlled. We propose this route as a universal approach for the deposition of large-area coatings of nanoporous silica with the potential for incorporating a broad variety of other dopant species. As for the present case, we observe, on the one hand, antireflective properties which enable the reduction of reflection losses from float glass by up to 3.7 percent points. On the other hand, the incorporation of nanoscale tungstic precipitates provides a lever for tailoring the coating hydrophilicity and, eventually, also surface acidity. This may provide a future route for combining optical performance with anti-fouling functionality.
- ItemTuning the magneto-optical response of TbPc2 single molecule magnets by the choice of the substrate(London [u.a.] : RSC, 2015) Robaschik, Peter; Fronk, Michael; Toader, Marius; Klyatskaya, Svetlana; Ganss, Fabian; Siles, Pablo F.; Schmidt, Oliver G.; Albrecht, Manfred; Hietschold, Michael; Ruben, Mario; Zahn, Dietrich R.T.; Salvan, GeorgetaIn this work, we investigated the magneto-optical response of thin films of TbPc2 on substrates which are relevant for (spin) organic field effect transistors (SiO2) or vertical spin valves (Co) in order to explore the possibility of implementing TbPc2 in magneto-electronic devices, the functionality of which includes optical reading. The optical and magneto-optical properties of TbPc2 thin films prepared by organic molecular beam deposition (OMBD) on silicon substrates covered with native oxide were investigated by variable angle spectroscopic ellipsometry (VASE) and magneto-optical Kerr effect (MOKE) spectroscopy at room temperature. The magneto-optical activity of the TbPc2 films can be significantly enhanced by one to two orders of magnitude upon changing the molecular orientation (from nearly standing molecules on SiO2/Si substrates to nearly lying molecules on perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) templated SiO2/Si substrates) or by using metallic ferromagnetic substrates (Co).