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- ItemHigh temperature behavior of rual thin films on piezoelectric CTGS and LGS substrates(Basel : MDPI AG, 2020) Seifert, M.This paper reports on a significant further improvement of the high temperature stability of RuAl thin films (110 nm) on the piezoelectric Ca3TaGa3Si2O14 (CTGS) and La3Ga5SiO14 (LGS) substrates. RuAl thin films with AlN or SiO2 cover layers and barriers to the substrate (each 20 nm), as well as a combination of both were prepared on thermally oxidized Si substrates, which serve as a reference for fundamental studies, and the piezoelectric CTGS, as well as LGS substrates. In somefilms, additional Al layers were added. To study their high temperature stability, the samples were annealed in air and in high vacuum up to 900 °C, and subsequently their cross-sections, phase formation, film chemistry, and electrical resistivity were analyzed. It was shown that on thermally oxidized Si substrates, all films were stable after annealing in air up to 800 °C and in high vacuum up to 900 °C. The high temperature stability of RuAl thin films on CTGS substrates was improved up to 900 °C in high vacuum by the application of a combined AlN/SiO2 barrier layer and up to 800 °C in air using a SiO2 barrier. On LGS, the films were only stable up to 600 °C in air; however, a single SiO2 barrier layer was sufficient to prevent oxidation during annealing at 900 °C in high vacuum.
- ItemWafer-level uniformity of atomic-layer-deposited niobium nitride thin films for quantum devices(New York, NY : Inst., 2021) Knehr, Emanuel; Ziegler, Mario; Linzen, Sven; Ilin, Konstantin; Schanz, Patrick; Plentz, Jonathan; Diegel, Marco; Schmidt, Heidemarie; Il’iche, Evgeni; Siegel, MichaelSuperconducting niobium nitride thin films are used for a variety of photon detectors, quantum devices, and superconducting electronics. Most of these applications require highly uniform films, for instance, when moving from single-pixel detectors to arrays with a large active area. Plasma-enhanced atomic layer deposition (ALD) of superconducting niobium nitride is a feasible option to produce high-quality, conformal thin films and has been demonstrated as a film deposition method to fabricate superconducting nanowire single-photon detectors before. Here, we explore the property spread of ALD-NbN across a 6-in. wafer area. Over the equivalent area of a 2-in. wafer, we measure a maximum deviation of 1% in critical temperature and 12% in switching current. Toward larger areas, structural characterizations indicate that changes in the crystal structure seem to be the limiting factor rather than film composition or impurities. The results show that ALD is suited to fabricate NbN thin films as a material for large-area detector arrays and for new detector designs and devices requiring uniform superconducting thin films with precise thickness control.
- ItemControlling Growth of Poly (Triethylene Glycol Acrylate-Co-Spiropyran Acrylate) Copolymer Liquid Films on a Hydrophilic Surface by Light and Temperature(Basel : MDPI, 2021) Ben-Miled, Aziz; Nabiyan, Afshin; Wondraczek, Katrin; Schacher, Felix H.; Wondraczek, LotharA quartz crystal microbalance with dissipation monitoring (QCM-D) was employed for in situ investigations of the effect of temperature and light on the conformational changes of a poly (triethylene glycol acrylate-co-spiropyran acrylate) (P (TEGA-co-SPA)) copolymer containing 12–14% of spiropyran at the silica–water interface. By monitoring shifts in resonance frequency and in acoustic dissipation as a function of temperature and illumination conditions, we investigated the evolution of viscoelastic properties of the P (TEGA-co-SPA)-rich wetting layer growing on the sensor, from which we deduced the characteristic coil-to-globule transition temperature, corresponding to the lower critical solution temperature (LCST) of the PTEGA part. We show that the coil-to-globule transition of the adsorbed copolymer being exposed to visible or UV light shifts to lower LCST as compared to the bulk solution: the transition temperature determined acoustically on the surface is 4 to 8 K lower than the cloud point temperature reported by UV/VIS spectroscopy in aqueous solution. We attribute our findings to non-equilibrium effects caused by confinement of the copolymer chains on the surface. Thermal stimuli and light can be used to manipulate the film formation process and the film’s conformational state, which affects its subsequent response behavior.
- ItemInfluence of Polycation Composition on Electrochemical Film Formation(Basel : MDPI, 2018) Schneider, Sabine; Janssen, Corinna; Klindtworth, Elisabeth; Mergel, Olga; Möller, Martin; Plamper, FelixThe effect of polyelectrolyte composition on the electrodeposition onto platinum is investigated using a counterion switching approach. Film formation of preformed polyelectrolytes is triggered by oxidation of hexacyanoferrates(II) (ferrocyanide), leading to polyelectrolyte complexes, which are physically crosslinked by hexacyanoferrate(III) (ferricyanide) ions due to preferential ferricyanide/polycation interactions. In this study, the electrodeposition of three different linear polyelectrolytes, namely quaternized poly[2-(dimethylamino)ethyl methacrylate] (i.e., poly{[2-(methacryloyloxy)ethyl]trimethylammonium chloride}; PMOTAC), quaternized poly[2-(dimethylamino)ethyl acrylate] (i.e., poly{[2-(acryloyloxy)ethyl]trimethylammonium chloride}; POTAC), quaternized poly[N-(3-dimethylaminopropyl)methacrylamide] (i.e., poly{[3-(methacrylamido)propyl]trimethylammonium chloride}; PMAPTAC) and different statistical copolymers of these polyelectrolytes with N-(3-aminopropyl)methacrylamide (APMA), are studied. Hydrodynamic voltammetry utilizing a rotating ring disk electrode (RRDE) shows the highest deposition efficiency DE for PMOTAC over PMAPTAC and over POTAC. Increasing incorporation of APMA weakens the preferred interaction of the quaternized units with the hexacyanoferrate(III) ions. At a sufficient APMA content, electrodeposition can thus be prevented. Additional electrochemical quartz crystal microbalance measurements reveal the formation of rigid polyelectrolyte films being highly crosslinked by the hexacyanoferrate(III) ions. Results indicate a different degree of water incorporation into these polyelectrolyte films. Hence, by adjusting the polycation composition, film properties can be tuned, while different chemistries can be incorporated into these electrodeposited thin hydrogel films.
- ItemAnalysis of electronic properties frommagnetotransport measurements on Ba(Fe1-xNix)2As2 thin films(Basel : MDPI AG, 2020) Shipulin, I.; Richter, S.; Thomas, A.A.; Nielsch, K.; Hühne, R.; Martovitsky, V.We performed a detailed structural, magnetotransport, and superconducting analysis of thin epitaxial Ba(Fe1-xNix)2As2 films with Ni doping of x = 0.05 and 0.08, as prepared by pulsed laser deposition. X-ray diffraction studies demonstrate the high crystalline perfection of the films, which have a similar quality to single crystals. Furthermore, magnetotransport measurements of the films were performed in magnetic fields up to 9 T. The results we used to estimate the density of electronic states at the Fermi level, the coefficient of electronic heat capacity, and other electronic parameters for this compound, in their dependence on the dopant concentration within the framework of the Ginzburg-Landau-Abrikosov-Gorkov theory. The comparison of the determined parameters with measurement data on comparable Ba(Fe1-xNix)2As2 single crystals shows good agreement, which confirms the high quality of the obtained films.
- ItemIncorporation of nitrogen into TiO2 thin films during PVD processes(Bristol : Institute of Physics Publishing, 2014) Asenova, I.; Manova, D.; Mändl, S.In this paper we investigate the possibility of incorporating nitrogen into amorphous, photocatalytic TiO2 thin films, prepared at room temperature, during the growth process. The aim is to reduce the bandgap of the UV active thin films. Physical vapor deposition experiments employing a titanium vacuum arc with gas backfill ranging from pure oxygen to pure nitrogen, are carried out. The resulting films are characterized for chemical composition, phase composition, optical properties and hydrophilicity in order to determine a correlation between gas composition and thin film properties. The experimental results point that a visible change in the band structure of the deposited layers is achieved.
- ItemFano-like resonances sustained by Si doped InAsSb plasmonic resonators integrated in GaSb matrix(Washington, DC : Optical Society of America, 2015) Taliercio, Thierry; Guilengui, Vilianne NTsame; Cerutti, Laurent; Rodriguez, Jean-Baptiste; Barho, Franziska; Rodrigo, Maria-José Milla; Gonzalez-Posada, Fernando; Tournié, Eric; Niehle, Michael; Trampert, AchimBy using metal-free plasmonics, we report on the excitation of Fano-like resonances in the mid-infrared where the Fano asymmetric parameter, q, varies when the dielectric environment of the plasmonic resonator changes. We use silicon doped InAsSb alloy deposited by molecular beam epitaxy on GaSb substrate to realize the plasmonic resonators exclusively based on semiconductors. We first demonstrate the possibility to realize high quality samples of embedded InAsSb plasmonic resonators into GaSb host using regrowth technique. The high crystalline quality of the deposited structure is confirmed by scanning transmission electron microscopy (STEM) observation. Second, we report Fano-like resonances associated to localized surface plasmons in both cases: uncovered and covered plasmonic resonators, demonstrating a strong line shape modification. The optical properties of the embedded structures correspond to those modeled by finite-difference time-domain (FDTD) method and by a model based on Fano-like line shape. Our results show that all-semiconductor plasmonics gives the opportunity to build new plasmonic structures with embedded resonators of highly doped semiconductor in a matrix of un-doped semiconductor for mid-IR applications.
- ItemGlow discharge optical emission spectrometry for quantitative depth profiling of CIGS thin-films(Cambridge : Royal Society of Chemistry, 2019) Kodalle, T.; Greiner, D.; Brackmann, V.; Prietzel, K.; Scheu, A.; Bertram, T.; Reyes-Figueroa, P.; Unold, T.; Abou-Ras, D.; Schlatmann, R.; Kaufmann, C.A.; Hoffmann, V.Determining elemental distributions dependent on the thickness of a sample is of utmost importance for process optimization in different fields e.g. from quality control in the steel industry to controlling doping profiles in semiconductor labs. Glow discharge optical emission spectrometry (GD-OES) is a widely used tool for fast measurements of depth profiles. In order to be able to draw profound conclusions from GD-OES profiles, one has to optimize the measurement conditions for the given application as well as to ensure the suitability of the used emission lines. Furthermore a quantification algorithm has to be implemented to convert the measured properties (intensity of the emission lines versus sputtering time) to more useful parameters, e.g. the molar fractions versus sample depth (depth profiles). In this contribution a typical optimization procedure of the sputtering parameters is adapted to the case of polycrystalline Cu(In,Ga)(S,Se)2 thin films, which are used as absorber layers in solar cell devices, for the first time. All emission lines used are shown to be suitable for the quantification of the depth profiles and a quantification routine based on the assumption of constant emission yield is used. The accuracy of this quantification method is demonstrated on the basis of several examples. The bandgap energy profile of the compound semiconductor, as determined by the elemental distributions, is compared to optical measurements. The depth profiles of Na-the main dopant in these compounds-are correlated with measurements of the open-circuit voltage of the corresponding devices, and the quantification of the sample depth is validated by comparison with profilometry and X-ray fluorescence measurements.
- ItemThe influence of Sb doping on the local structure and disorder in thermoelectric ZnO:Sb thin films(Lausanne : Elsevier, 2023) Ribeiro, Joana M.; Rodrigues, Frederico J.; Correia, Filipe C.; Pudza, Inga; Kuzmin, Alexei; Kalinko, Aleksandr; Welter, Edmund; Barradas, Nuno P.; Alves, Eduardo; LaGrow, Alec P.; Bondarchuk, Oleksandr; Welle, Alexander; Telfah, Ahmad; Tavares, Carlos J.Thermoelectric transparent ZnO:Sb thin films were deposited by magnetron sputtering, with Sb content varying between 2 and 14 at%. As evidenced by X-ray diffraction analysis, the films crystallize in the ZnO wurtzite structure for lower levels of Sb-doping, developing a degree of amorphization for higher levels of Sb-doping. Temperature-dependent (10–300 K) X-ray absorption spectroscopy studies of the produced thin films were performed at the Zn and Sb K-edges to shed light on the influence of Sb doping on the local atomic structure and disorder in the ZnO:Sb thin films. The analysis of the Zn K-edge EXAFS spectra by the reverse Monte Carlo method allowed to extract detailed and accurate structural information in terms of the radial and bond angle distribution functions. The obtained results suggest that the introduction of antimony to the ZnO matrix promotes static disorder, which leads to partial amorphization with very small crystallites (∼3 nm) for large (12–14 at%) Sb content. Rutherford backscattering spectrometry (RBS) experiments enabled the determination of the in-depth atomic composition profiles of the films. The film composition at the surfaces determined by X-ray photoelectron spectroscopy (XPS) matches that of the bulk determined by RBS, except for higher Sb-doping in ZnO films, where the concentration of oxygen determined by XPS is smaller near the surface, possibly due to the formation of oxygen vacancies that lead to an increase in electrical conductivity. Traces of Sb–Sb metal bonds were found by XPS for the sample with the highest level of Sb-doping. Time-of-flight secondary ion mass spectrometry obtained an Sb/Zn ratio that follows that of the film bulk determined by RBS, although Sb is not always homogeneous, with samples with smaller Sb content (2 and 4 at% of Sb) showing a larger Sb content closer to the film/substrate interface. From the optical transmittance and reflectance curves, it was determined that the films with the lower amount of Sb doping have larger optical band-gaps, in the range of 2.9–3.2 eV, while the partially amorphous films with higher Sb content have smaller band-gaps in the range of 1.6–2.1 eV. Albeit the short-range crystalline order (∼3 nm), the film with 12 at% of Sb has the highest absolute Seebeck coefficient (∼56 μV/K) and a corresponding thermoelectric power factor of ∼0.2 μW·K−2·m−1.
- ItemEpitaxial synthesis of unintentionally doped p-type SnO (001) via suboxide molecular beam epitaxy(Melville, NY : AIP, 2023) Egbo, Kingsley; Luna, Esperanza; Lähnemann, Jonas; Hoffmann, Georg; Trampert, Achim; Grümbel, Jona; Kluth, Elias; Feneberg, Martin; Goldhahn, Rüdiger; Bierwagen, OliverBy employing a mixed SnO2 + Sn source, we demonstrate suboxide molecular beam epitaxy (S-MBE) growth of phase-pure single-crystalline metastable SnO (001) thin films on Y-stabilized ZrO2 (001) substrates at a growth rate of ∼1.0 nm/min without the need for additional oxygen. These films grow epitaxially across a wide substrate temperature range from 150 to 450 °C. Hence, we present an alternative pathway to overcome the limitations of high Sn or SnO2 cell temperatures and narrow growth windows encountered in previous MBE growth of metastable SnO. In situ laser reflectometry and line-of-sight quadrupole mass spectrometry were used to investigate the rate of SnO desorption as a function of substrate temperature. While SnO ad-molecule desorption at TS = 450 °C was growth-rate limiting, the SnO films did not desorb at this temperature after growth in vacuum. The SnO (001) thin films are transparent and unintentionally p-type doped, with hole concentrations and mobilities in the range of 0.9-6.0 × 1018 cm-3 and 2.0-5.5 cm2 V-1 s-1, respectively. These p-type SnO films obtained at low substrate temperatures are promising for back-end-of-line (BEOL) compatible applications and for integration with n-type oxides in pn heterojunctions and field-effect transistors.
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