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  • 1.
    Ali, Sharafat
    et al.
    Linnaeus Univ, Sweden.
    Magnusson, Roger
    Linnaeus Univ, Sweden.
    Pshyk, Oleksandr
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Empa Swiss Fed Labs Mat Sci & Technol, Switzerland.
    Birch, Jens
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Eklund, Per
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Le Febvrier, Arnaud
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Effect of O/N content on the phase, morphology, and optical properties of titanium oxynitride thin films2023In: Journal of Materials Science, ISSN 0022-2461, E-ISSN 1573-4803, Vol. 58, p. 10975-10985Article in journal (Refereed)
    Abstract [en]

    Phase formation, morphology, and optical properties of Ti(O,N) thin films with varied oxygen-to- nitrogen ration content were investigated. The films were deposited by magnetron sputtering at 500 & DEG;C on Si(100) and c-plane sapphire substrate. A competition between a NaCl B1 structure TiN1-xOx, a rhombohedral structure Ti-2(O1-yNy)(3), and an anatase structure Ti(O1-zNz)(2) phase was observed. While the N-rich films were composed of a NaCl B1 TiN1-xOx phase, an increase of oxygen in the films yields the growth of rhombohedral Ti-2(O1-yNy)(3) phase and the oxygen-rich films are comprised of a mixture of the rhombohedral Ti-2(O1-yNy)(3) phase and anatase Ti(O1-zNz)(2) phase. The optical properties of the films were correlated to the phase composition and the observation of abrupt changes in terms of refractive index and absorption coefficient. The oxide film became relatively transparent in the visible range while the addition of nitrogen into films increases the absorption. The oxygen rich-samples have bandgap values below 3.75 eV, which is higher than the value for pure TiO2, and lower than the optical bandgap of pure TiN. The optical properties characterizations revealed the possibility of adjusting the band gap and the absorption coefficient depending on the N-content, because of the phases constituting the films combined with anionic substitution.

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  • 2.
    Greczynski, Grzegorz
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Pshyk, Oleksandr
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Medicine and Health Sciences.
    Hultman, Lars
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Toward an increased reliability of chemical bonding assignment in insulating samples by x-ray photoelectron spectroscopy2023In: Science Advances, E-ISSN 2375-2548, Vol. 9, no 37, article id eadi3192Article in journal (Refereed)
    Abstract [en]

    X-ray photoelectron spectroscopy (XPS) spectra from solid samples are conventionally referenced to the spectrometer Fermi level (FL). While, in the case of metallic samples, alignment of the sample and the spectrometer FLs can be directly verified from the measured Fermi edge position, thus allowing to assess the surface electrical potential, this is not a workable option for insulators. When applied, it generates a large spread in reported binding energy values that often exceed involved chemical shifts. By depositing insulating amorphous alumina thin films on a variety of conducting substrates with different work functions, we show not only that FL referencing fails but also that the Al2O3 energy levels align instead to the vacuum level, as postulated in the early days of XPS. Based on these model experiments that can be repeated for all sorts of thin-film insulators, a solution to the binding energy reference problem is proposed for reliable assessment of chemical bonding.

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  • 3.
    Pshyk, Oleksandr
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Petrov, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Univ Illinois, IL 61801 USA; Natl Taiwan Univ Sci & Technol, Taiwan.
    Bakhit, Babak
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Lu, Jun
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Hultman, Lars
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Greczynski, Grzegorz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Energy-efficient physical vapor deposition of dense and hard Ti-Al-W-N coatings deposited under industrial conditions2023In: Materials & design, ISSN 0264-1275, E-ISSN 1873-4197, Vol. 227, article id 111753Article in journal (Refereed)
    Abstract [en]

    Decreasing the growth temperature to lower energy consumption and enable deposition on temperature-sensitive substrates during thin film growth by magnetron sputtering is crucial for sustainable develop-ment. High-mass metal ion irradiation of the growing film surface with ion energy controlled by metal-ion-synchronized biasing, allows to replace conventionally-used resistive heating, as was recently demonstrated in experiments involving a hybrid high-power impulse and dc magnetron co-sputtering (HiPIMS/DCMS) setup and stationary substrates. Here, we report the extension of the method to indus-trial scale conditions. As a model-case towards understanding the role of one-fold substrate rotation on Ti0.50Al0.50N film growth employing W irradiation, we investigate the effect of two parameters: W ion energy (controlled in the range 45 <= EW <= 630 eV by the amplitude of synchronized substrate bias voltage) and W ion dose per deposited metal atom (determined by the target power). We show that the efficient densification of coatings grown without external heating can be achieved by minimizing the thickness of DCMS-deposited Ti0.50Al0.50N layer that is exposed to an W ion flux, or by increasing EW, at a given Ti0.50Al0.50N thickness.(c) 2023 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).

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  • 4.
    Pshyk, Oleksandr V.
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Li, Xiao
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Petrov, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Materials Research Laboratory, University of Illinois, Urbana, IL, United States.
    Sangiovanni, Davide Giuseppe
    Linköping University, Department of Physics, Chemistry and Biology, Theoretical Physics. Linköping University, Faculty of Science & Engineering.
    Palisaitis, Justinas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Hultman, Lars
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Greczynski, Grzegorz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Discovery of Guinier-Preston zone hardening in refractory nitride ceramics2023In: Acta Materialia, ISSN 1359-6454, E-ISSN 1873-2453, Vol. 255, article id 119105Article in journal (Refereed)
    Abstract [en]

    Traditional age hardening mechanisms in refractory ceramics consist of precipitation of fine particles. These processes are vital for widespread wear-resistant coating applications. Here, we report novel Guinier-Preston zone hardening, previously only known to operate in soft light-metal alloys, taking place in refractory ceramics like multicomponent nitrides. The added superhardening, discovered in thin films of Ti-Al-W-N upon high temperature annealing, comes from the formation of atomic-plane-thick W disks populating {111} planes of the cubic matrix, as observed by atomically resolved high resolution scanning transmission electron microscopy and corroborated by ab initio calculations and molecular dynamics simulations. Guinier-Preston zone hardening concurrent with spinodal decomposition is projected to exist in a range of other ceramic solid solutions and thus provides a new approach for the development of advanced materials with outstanding mechanical properties and higher operational temperature range for the future demanding applications.

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  • 5.
    Rogoz, Vladyslav
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Sumy State Univ, Ukraine.
    Pshyk, Oleksandr
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Medicine and Health Sciences. Empa Swiss Fed Labs Mat Sci & Technol, Switzerland.
    Wicher, Bartosz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Warsaw Univ Technol, Poland.
    Palisaitis, Justinas
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Lu, Jun
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Primetzhofer, Daniel
    Uppsala Univ, Sweden.
    Petrov, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Univ Illinois, IL 61801 USA.
    Hultman, Lars
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Greczynski, Grzegorz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    High-mass metal ion irradiation enables growth of high-entropy sublattice nitride thin films from elemental targets2023In: Journal of Vacuum Science & Technology. A. Vacuum, Surfaces, and Films, ISSN 0734-2101, E-ISSN 1520-8559, Vol. 41, no 6, article id 063108Article in journal (Refereed)
    Abstract [en]

    Synthesis of high-entropy sublattice nitride (HESN) coatings by magnetron sputtering is typically done using custom-made alloyed targets with specific elemental compositions. This approach is expensive, requires long delivery times, and offers very limited flexibility to adjust the film composition. Here, we demonstrate a new method to grow HESN films, which relies on elemental targets arranged in the multicathode configuration with substrates rotating during deposition. TiVNbMoWN films are grown at a temperature of similar to 520(degrees)C using Ti, V, Nb, and Mo targets operating in the direct current magnetron sputtering mode, while the W target, operated by high power impulse magnetron sputtering (HiPIMS), provides a source of heavy ions. The energy of the metal ions EW+ is controlled in the range from 80 to 620 eV by varying the amplitude of the substrate bias pulses V-s, synchronized with the metal-ion-rich phase of HiPIMS pulses. We demonstrate that W(+ )irradiation provides dynamic recoil mixing of the film-forming components in the near-surface atomic layers. For EW+ >= 320 eV the multilayer formation phenomena, inherent for this deposition geometry, are suppressed and, hence, compositionally uniform HESN films are obtained, as confirmed by the microstructural and elemental analysis.(c) 2023 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license(http://creativecommons.org/licenses/by/4.0/)

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  • 6.
    Wicher, Bartosz
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Warsaw Univ Technol, Poland.
    Chodun, Rafal
    Warsaw Univ Technol, Poland.
    Greczynski, Grzegorz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Lachowski, Artur
    Polish Acad Sci, Poland.
    Trzcinski, Marek
    Bydgoszcz Univ Sci & Technol, Poland.
    Pshyk, Oleksandr
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Krol, Krystian
    Warsaw Univ Technol, Poland.
    Kulikowski, Krzysztof
    Warsaw Univ Technol, Poland.
    Skowronski, Lukasz
    Bydgoszcz Univ Sci & Technol, Poland.
    Zdunek, Krzysztof
    Warsaw Univ Technol, Poland.
    Carbon ion self-sputtering attained by sublimation of hot graphite target and controlled by pulse injection of a neon-helium gas mixture2023In: Applied Surface Science, ISSN 0169-4332, E-ISSN 1873-5584, Vol. 620, article id 156708Article in journal (Refereed)
    Abstract [en]

    The operation of graphite targets with an increased temperature (HT - hot target) is studied for the case of gas injection magnetron sputtering (GIMS) of: 1) diamond-like carbon (DLC), and 2) carbon-silicon carbide (C-SiC) films. A purposely-thinned graphite target with a reduced thermal conductivity is applied for DLC deposition, extending its high temperature sputtering range up to 1636 degrees C. For the purpose of C-SiC synthesis four sockets with a silicon carbide powder are designed within graphite target. In this approach, the C-SiC target surface can be heated up to 1443 degrees C due to a greater energy input from impulse plasma, in the range 322-932 J. The HT sputtering is energy-controlled by a pulsed injection of a neon-helium gas mixture. High-energy Ne+ and He+ ions extend the length of pulsed GIMS discharge due to the self-sputtering effect observed during the deposition of DLC and C-SiC films. These conditions result in an almost 5-fold increase in the film growth rate (up to 185 nm/min) with respect to the operation with a cold target, which is due to the assisting vapour sublimation from custom-designed graphite-based targets. The temperature boosted HT GIMS discharge, proves to be an efficient tool for reaching relatively high (similar to 35 %) sp(3)-hybridized C content in both carbon-based materials. It also allows for tailoring the energy bandgap of DLC-based optical structure, in the range from 1.7 to 2.75 eV, due to the formation of the (C-C) and (C-O) bonds. Higher content of silicon oxide (SiO2-x) and silicon carbide (SiC) phases (15 - 23 %) in the case of C-SiC films results in hardness increase from 21.8 to 30.1 GPa.

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  • 7.
    Wicher, Bartosz
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Warsaw Univ Technol, Poland.
    Pshyk, Oleksandr
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Empa Swiss Fed Labs Mat Sci & Technol, Switzerland.
    Li, Xiao
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Bakhit, Babak
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Rogoz, Vladyslav
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Petrov, Ivan
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering. Univ Illinois, IL 61801 USA.
    Hultman, Lars
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Greczynski, Grzegorz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Superhard oxidation-resistant Ti1-xAlxBy thin films grown by hybrid HiPIMS/DCMS co-sputtering diboride targets without external substrate heating2024In: Materials & design, ISSN 0264-1275, E-ISSN 1873-4197, Vol. 238, article id 112727Article in journal (Refereed)
    Abstract [en]

    Ti1-xAlxBy films (0.40 <= x <= 0.76, and 1.81 <= y <= 2.03) combining good mechanical properties and high-temperature oxidation resistance are demonstrated. Layers are grown using a hybrid high-power impulse and dc magnetron co-sputtering employing two target configurations (AlB2-HiPIMS/TiB2-DCMS and TiB2-HiPIMS/AlB2-DCMS) and no external substrate heating. Near-stoichiometric B content are achieved by co-sputtering two diboride targets. Time-resolved ion mass spectrometry analyses reveal that the ionization of the DCMS flux (Al) is much higher during TiB2-HiPIMS/AlB2-DCMS. The effect is caused by the difference in the first ionization potentials and the ionization probabilities of sputtered metals and results in lower B/metal ratios in films grown in this configuration. The B/metal ratio in the single-phase Ti1-xAlxBy decreases with increasing Al content, which is explained by the change between angular distribution of Ti and Al atoms. Alloying with Al improves the high-temperature oxidation resistance: the thickness of the oxide-scale forming after 1 h anneal at 800 degrees C decreases more than 15 times upon increasing x from 0.36 to 0.74. Ti1-xAlxBy films with 0.58 <= x <= 0.67 offer the best compromise between high-temperature oxidation resistance and mechanical properties with an average oxide scale thickness 90-180 nm and the hardness of 34-38 GPa.

  • 8.
    Wu, Zhixing
    et al.
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Vagin, Mikhail
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Boyd, Robert
    Linköping University, Department of Physics, Chemistry and Biology, Plasma and Coating Physics. Linköping University, Faculty of Science & Engineering.
    Ding, Penghui
    Linköping University, Department of Science and Technology, Laboratory of Organic Electronics. Linköping University, Faculty of Science & Engineering.
    Pshyk, Oleksandr
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Greczynski, Grzegorz
    Linköping University, Department of Physics, Chemistry and Biology, Thin Film Physics. Linköping University, Faculty of Science & Engineering.
    Odén, Magnus
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Björk, Emma
    Linköping University, Department of Physics, Chemistry and Biology, Nanostructured Materials. Linköping University, Faculty of Science & Engineering.
    Selectivity Control of Oxygen Reduction Reaction over Mesoporous Transition Metal Oxide Catalysts for Electrified Purification Technologies2023In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 15, no 21, p. 26093-26103Article in journal (Refereed)
    Abstract [en]

    Direct electrification of oxygen-associated reactionscontributesto large-scale electrical storage and the launch of the green hydrogeneconomy. The design of the involved catalysts can mitigate the electricalenergy losses and improve the control of the reaction products. Weevaluate the effect of the interface composition of electrocatalystson the efficiency and productivity of the oxygen reduction reaction(ORR) and oxygen evolution reaction (OER), both mechanistically andat device levels. The ORR and OER were benchmarked on mesoporous nickel-(II)oxide and nickel cobaltite (NiO and NiCo2O4,respectively) obtained by a facile template-free hydrothermal synthesis.Physicochemical characterization showed that both NiO and NiCo2O4 are mesoporous and have a cubic crystal structurewith abundant surface hydroxyl species. NiCo2O4 showed higher electrocatalytic activity in OER and selectivity towater as the terminal product of ORR. On the contrary, ORR over NiOyielded hydroxyl radicals as products of a Fenton-like reaction ofH(2)O(2). The product selectivity in ORR was usedto construct two electrolyzers for electrified purification of oxygenand generation of hydroxyl radicals.

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