TRR 87:  Pulsed High Power Plasmas for the Synthesis of Nanostructural Functional Layers

• Subject Area: Computer Science, Systems and Electrical Engineering ; Chemistry ; Mechanical and Industrial Engineering ; Materials Science and Engineering ; Physics
• Term: from 2010 to 2022
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 138690629

• Final Report Year: 2023

Final Report Abstract

Fundamental phenomena in high power pulsed plasmas used for coating by magnetron sputtering of ceramic layers and by plasma enhanced chemical vapor deposition (PECVD) of SiO2 barrier and membrane layers have been elucidated by a combination of very detailed experiments combined with theory and simulation. In the field of pulsed magnetron plasmas, dynamic ionization zones favoring plasma transport from the target to the substrate were observed and characterized. The mechanism of action was identified by synchronized measurements consistent with theory and simulation. Scaling to large industrial facilities was demonstrated. Large-scale multifrequency plasmas were set up for the deposition of ceramic coatings, quantitatively characterized and simulated, and ultimately optimized. In the process, the coupling of the different frequencies and the spatial expansion of the plasmas were elucidated in alignment with simulation and theory. Finally, by screening the correlation between plasma properties and layer properties, it was possible to develop extended structure zone diagrams. In the field of PECVD and plasma enhanced atomic layer deposition (PE-ALD), the entire chain from substrate pretreatment, deposition of an intermediate layer and deposition of the actual barrier layer was elucidated and described in detail. Many, often quantitative, individual experiments were able to dispel a number of ideas previously assumed to be valid, re-evaluate them and integrate them into the overall process. Building on the wealth of experience, it was also possible in the final phase to realize the process of depositing membrane layers, which is the inverse of barrier deposition. This also succeeded exceptionally well and quickly due to the quantitative characterization of all relevant parameters. As gas separation seems to play an increasingly important role, the foundations for many further research projects were laid here.

Publications

• Combined in situ FTIR-spectroscopic and electrochemical analysis of nanopores in ultra-thin SiOx-like plasma polymer barrier films. Journal of Physics D: Applied Physics, 46(8), 084015.
  Liu, C.-N.; Ozkaya, B.; Steves, S.; Awakowicz, P. & Grundmeier, G.
  
• Influence of HPPMS pulse length and inert gas mixture on the properties of (Cr,Al)N coatings. Thin Solid Films, 549, 192-198.
  Bagcivan, N.; Bobzin, K.; Grundmeier, G.; Wiesing, M.; Ozcan, O.; Kunze, C. & Brugnara, R.H.
  
• Influence of layer type and order on barrier properties of multilayer PECVD barrier coatings. Journal of Physics D: Applied Physics, 47(1), 015201.
  Bahroun, K.; Behm, H.; Mitschker, F.; Awakowicz, P.; Dahlmann, R. & Hopmann, Ch
  
• Silicon oxide barrier films deposited on PET foils in pulsed plasmas: influence of substrate bias on deposition process and film properties. Journal of Physics D: Applied Physics, 46(8), 084013.
  Steves, S.; Ozkaya, B.; Liu, C.-N.; Ozcan, O.; Bibinov, N.; Grundmeier, G. & Awakowicz, P.
  
• Surface pre-treatment for barrier coatings on polyethylene terephthalate. Journal of Physics D: Applied Physics, 46(8), 084012.
  Bahre, H.; Bahroun, K.; Behm, H.; Steves, S.; Awakowicz, P.; Böke, M.; Hopmann, Ch & Winter, J.
  
• Electrochemical analysis of strain-induced crack formation of bilayer barrier plasma polymer films on metal and polymer substrates. Surface and Coatings Technology, 244, 173-179.
  Ozkaya, B.; Bahre, H.; Böke, M.; Höwer, D.; Reese, S.; Winter, J. & Grundmeier, G.
  
• Influence of Ar/Kr ratio and pulse parameters in a Cr-N high power pulse magnetron sputtering process on plasma and coating properties. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, 32(2).
  Bobzin, Kirsten; Bagcivan, Nazlim; Theiß, Sebastian; Trieschmann, Jan; Brugnara, Ricardo Henrique; Preissing, Sven & Hecimovic, Ante
  
• Film Stress of Amorphous Hydrogenated Carbon on Biaxially Oriented Polyethylene Terephthalate. Plasma Processes and Polymers, 12(9), 896-904.
  Bahre, Hendrik; Behm, Henrik; Grochla, Dario; Böke, Marc; Dahlmann, Rainer; Hopmann, Christian; Ludwig, Alfred & Winter, Jörg
  
• An efficient PE-ALD process for TiO2 thin films employing a new Ti-precursor. Journal of Materials Chemistry C, 4(5), 1057-1065.
  Gebhard, M.; Mitschker, F.; Wiesing, M.; Giner, I.; Torun, B.; de los Arcos, T.; Awakowicz, P.; Grundmeier, G. & Devi, A.
  
• On the physics of a large CCP discharge. Plasma Sources Science and Technology, 25(2), 025020.
  Eremin, D.; Bienholz, S.; Szeremley, D.; Trieschmann, J.; Ries, S.; Awakowicz, P.; Mussenbrock, T. & Brinkmann, R. P.
  
• The effect of UV radiation from oxygen and argon plasma on the adhesion of organosilicon coatings on polypropylene. Journal of Physics D: Applied Physics, 50(1), 015201.
  Jaritz, M.; Behm, H.; Hopmann, Ch; Kirchheim, D.; Mitschker, F.; Awakowicz, P. & Dahlmann, R.
  
• From quantum to continuum mechanics: studying the fracture toughness of transition metal nitrides and oxynitrides. Materials Research Letters, 6(2), 142-151.
  Gibson, James S. K.-L.; Rezaei, Shahed; Rueß, Holger; Hans, Marcus; Music, Denis; Wulfinghoff, Stephan; Schneider, Jochen M.; Reese, Stefanie & Korte-Kerzel, Sandra
  
• Influence of organic surface chemistry on the nucleation of plasma deposited SiOxfilms. Journal of Physics D: Applied Physics, 50(20), 204002.
  Hoppe, C.; Mitschker, F.; Giner, I.; de los Arcos, T.; Awakowicz, P. & Grundmeier, G.
  
• Influence of PE-CVD and PE-ALD on defect formation in permeation barrier films on PET and correlation to atomic oxygen fluence. Journal of Physics D: Applied Physics, 50(23), 235201.
  Mitschker, F.; Steves, S.; Gebhard, M.; Rudolph, M.; Schücke, L.; Kirchheim, D.; Jaritz, M.; Brochhagen, M.; Hoppe, Ch; Dahlmann, R.; Böke, M.; Benedikt, J.; Giner, I.; de los Arcos, T.; Hopmann, Ch; Grundmeier, G.; Devi, A. & Awakowicz, P.
  
• Influence of residual stress on the adhesion and surface morphology of PECVD-coated polypropylene. Journal of Physics D: Applied Physics, 50(44), 445301.
  Jaritz, Montgomery; Hopmann, Christian; Behm, Henrik; Kirchheim, Dennis; Wilski, Stefan; Grochla, Dario; Banko, Lars; Ludwig, Alfred; Böke, Marc; Winter, Jörg; Bahre, Hendrik & Dahlmann, Rainer
  
• Analysis of dispersive interactions at polymer/TiAlN interfaces by means of dynamic force spectroscopy. Physical Chemistry Chemical Physics, 20(1), 180-190.
  Wiesing, M.; de los Arcos, T.; Gebhard, M.; Devi, A. & Grundmeier, G.
  
• Improved homogeneity of plasma and coating properties using a lance matrix gas distribution in MW-PECVD. Journal of Coatings Technology and Research, 16(2), 573-583.
  Kirchheim, Dennis; Wilski, Stefan; Jaritz, Montgomery; Mitschker, Felix; Oberberg, Moritz; Trieschmann, Jan; Banko, Lars; Brochhagen, Markus; Schreckenberg, Rabea; Hopmann, Christian; Böke, Marc; Benedikt, Jan; de los Arcos, Teresa; Grundmeier, Guido; Grochla, Dario; Ludwig, Alfred; Mussenbrock, Thomas; Brinkmann, Ralf Peter; Awakowicz, Peter & Dahlmann, Rainer
  
• Influence of spokes on the ionized metal flux fraction in chromium high power impulse magnetron sputtering. Journal of Physics D: Applied Physics, 51(11), 115201.
  Biskup, B.; Maszl, C.; Breilmann, W.; Held, J.; Böke, M.; Benedikt, J. & von, Keudell A.
  
• PEALD of SiO2 and Al2O3 Thin Films on Polypropylene: Investigations of the Film Growth at the Interface, Stress, and Gas Barrier Properties of Dyads. ACS Applied Materials & Interfaces, 10(8), 7422–7434.
  Gebhard, Maximilian; Mai, Lukas; Banko, Laes; Mitschker, Felix; Hoppe, Christian; Jaritz, Montgomery; Kirchheim, Dennis; Zekorn, Christoph; de los Arcos, Teresa; Grochla, Dario; Dahlmann, Rainer; Grundmeier, Guido; Awakowicz, Peter; Ludwig, Alfred & Devi, Anjana
  
• Atomistically motivated interface model to account for coupled plasticity and damage at grain boundaries. Journal of the Mechanics and Physics of Solids, 124, 325-349.
  Rezaei, Shahed; Jaworek, David; Mianroodi, Jaber Rezaei; Wulfinghoff, Stephan & Reese, Stefanie
  
• Ion energy control via the electrical asymmetry effect to tune coating properties in reactive radio frequency sputtering. Plasma Sources Science and Technology, 28(11), 114001.
  Ries, Stefan; Banko, Lars; Hans, Marcus; Primetzhofer, Daniel; Schneider, Jochen M.; Ludwig, Alfred; Awakowicz, Peter & Schulze, Julian
  
• Characterisation of micropores in plasma deposited SiO x films by means of positron annihilation lifetime spectroscopy. Journal of Physics D: Applied Physics, 53(47), 475205.
  Hoppe, C.; Mitschker, F.; Butterling, M.; Liedke, M. O.; de Los Arcos, T.; Awakowicz, P.; Wagner, A. & Grundmeier, G.
  
• Electron density, temperature and the potential structure of spokes in HiPIMS. Plasma Sources Science and Technology, 29(2), 025006.
  Held, J.; Maaß, P. A.; Gathen, V. Schulz-von der & Keudell, A. von
  
• From Precursor Chemistry to Gas Sensors: Plasma‐Enhanced Atomic Layer Deposition Process Engineering for Zinc Oxide Layers from a Nonpyrophoric Zinc Precursor for Gas Barrier and Sensor Applications. Small, 16(22).
  Mai, Lukas; Mitschker, Felix; Bock, Claudia; Niesen, Alessia; Ciftyurek, Engin; Rogalla, Detlef; Mickler, Johannes; Erig, Matthias; Li, Zheshen; Awakowicz, Peter; Schierbaum, Klaus & Devi, Anjana
  
• How self-assembled organophosphonic acid monolayers on Ti0.5Al0.5N hard coatings affect the adsorption of polycarbonate melt. Applied Surface Science, 513, 145701.
  Theile-Rasche, C.; Wiesing, M.; Schwiderek, S.; Noeske, M. & Grundmeier, G.
  
• Predicting structure zone diagrams for thin film synthesis by generative machine learning. Communications Materials, 1(1).
  Banko, Lars; Lysogorskiy, Yury; Grochla, Dario; Naujoks, Dennis; Drautz, Ralf & Ludwig, Alfred
  
• Quantum-mechanical study of interaction between polycarbonate and M0.5Al0.5N(001) surfaces (M=Ti, V, Cr). Applied Surface Science, 520, 146306.
  Music, Denis; Rueß, Holger & Schneider, Jochen M.
  
• Single-Molecule Desorption Studies of Poly(acrylic acid) at Electrolyte/Oxide/TiAlN Interfaces. Langmuir, 36(32), 9489-9498.
  Schwiderek, Sabrina; Orive, Alejandro G.; Karimi, Aghda Soheil; Schneider, Jochen M.; de los Arcos, Teresa & Grundmeier, Guido
  
• Crystallography companion agent for high-throughput materials discovery. Nature Computational Science, 1(4), 290-297.
  Maffettone, Phillip M.; Banko, Lars; Cui, Peng; Lysogorskiy, Yury; Little, Marc A.; Olds, Daniel; Ludwig, Alfred & Cooper, Andrew I.
  
• Design of a TiAlON multilayer coating: Oxidation stability and deformation behavior. Surface and Coatings Technology, 421, 127417.
  Bobzin, K.; Kalscheuer, C.; Grundmeier, G.; de los Arcos, T.; Schwiderek, S. & Carlet, M.
  
• Direction-dependent fracture in solids: Atomistically calibrated phase-field and cohesive zone model. Journal of the Mechanics and Physics of Solids, 147, 104253.
  Rezaei, Shahed; Mianroodi, Jaber Rezaei; Brepols, Tim & Reese, Stefanie
  
• Multi-diagnostic experimental validation of 1d3v PIC/MCC simulations of low pressure capacitive RF plasmas operated in argon. Plasma Sources Science and Technology, 30(10), 105003.
  Schulenberg, David A.; Korolov, Ihor; Donkó, Zoltán; Derzsi, Aranka & Schulze, Julian
  
• Unravelling the ion-energy-dependent structure evolution and its implications for the elastic properties of (V,Al)N thin films. Acta Materialia, 214, 117003.
  Karimi, Aghda Soheil; Music, Denis; Unutulmazsoy, Yeliz; Sua, Heng Han; Mráz, Stanislav; Hans, Marcus; Primetzhofer, Daniel; Anders, André & Schneider, Jochen M.
  
• An energy-and charge-conserving electrostatic implicit particle-in-cell algorithm for simulations of collisional bounded plasmas. Journal of Computational Physics, 452, 110934.
  Eremin, D.
  
• Bond formation at polycarbonate | X interfaces (X=Ti, Al, TiAl) probed by X-ray photoelectron spectroscopy and density functional theory molecular dynamics simulations. Applied Surface Science, 593, 153363.
  Patterer, Lena; Ondračka, Pavel; Bogdanovski, Dimitri; Jende, Leonie; Prünte, Stephan; Mráz, Stanislav; Karimi, Aghda Soheil; Stelzer, Bastian; Momma, Markus & Schneider, Jochen M.
  
• Challenges in the interpretation of gas core levels for the determination of gas-solid interactions within dielectric porous films by ambient pressure XPS. Applied Surface Science, 604, 154525.
  de los Arcos, Teresa; Weinberger, Christian; Zysk, Frederik; Raj, Damerla Varun; Kollmann, Sabrina; Vieth, Pascal; Tiemann, Michael; Kühne, Thomas D. & Grundmeier, Guido
  
• Evaluation of the membrane performance of ultra-smooth silicon organic coatings depending on the process energy density. Thin Solid Films, 748, 139169.
  Kleines, Lara; Wilski, Stefan; Alizadeh, Philipp; Rubner, Jens; Wessling, Matthias; Hopmann, Christian & Dahlmann, Rainer
  
• From cathode to substrate: Plasma diagnostics on high power pulsed magnetron sputtering deposition of titanium nitride. Thin Solid Films, 755, 139331.
  Bobzin, K.; Kalscheuer, C.; Carlet, M. & Schulze, C.
  
• Hybrid reactive sputtering of transition metal aluminum oxynitrides. Thin Solid Films, 742, 139028.
  Bobzin, K.; Kalscheuer, C.; Carlet, M. & Schulze, C.
  
• Influence of different ester side groups in polymers on the vapor phase infiltration with trimethyl aluminum. Dalton Transactions, 51(4), 1384-1394.
  Mai, Lukas; Maniar, Dina; Zysk, Frederik; Schöbel, Judith; Kühne, Thomas D.; Loos, Katja & Devi, Anjana
  
• Influence of surface activation on the microporosity of PE‐CVD and PE‐ALD SiOx thin films on PDMS. Plasma Processes and Polymers, 19(4).
  Hoppe, Christian; Mitschker, Felix; Mai, Lukas; Liedke, Maciej Oskar; de los Arcos, Teresa; Awakowicz, Peter; Devi, Anjana; Attallah, Ahmed Gamal; Butterling, Maik; Wagner, Andreas & Grundmeier, Guido
  
• Ion-induced secondary electron emission of oxidized nickel and copper studied in beam experiments. Plasma Sources Science and Technology, 31(2), 025017.
  Buschhaus, R.; Prenzel, M. & von, Keudell A.
  
• Orientation dependence of the fracture mechanisms in (V,Al)N coatings determined by micropillar compression. Journal of Materials Research, 37(4), 1003-1017.
  Schoof, Markus R.; Gibson, James S. K.-L.; Karimi, Aghda Soheil; Hans, Marcus; Schneider, Jochen M. & Korte-Kerzel, Sandra
  
• Oxidation stability of chromium aluminum oxynitride hard coatings. Surface and Coatings Technology, 449, 128927.
  Bobzin, K.; Kalscheuer, C.; Grundmeier, G.; de los Arcos, T.; Kollmann, S. & Carlet, M.
  
• Charge-optimized many-body interaction potential for AlN revisited to explore plasma–surface interactions. Scientific Reports, 13(1).
  Gergs, Tobias; Mussenbrock, Thomas & Trieschmann, Jan
  
• Collisionless dissipation at the boundary sheath of magnetized low temperature plasmas. Plasma Sources Science and Technology, 32(4), 045011.
  Krüger, Dennis; Köhn, Kevin; Xu, Liang; Eremin, Denis & Brinkmann, Ralf Peter
  
• Ion kinetic energy-and ion flux-dependent mechanical properties and thermal stability of (Ti,Al)N thin films. Acta Materialia, 250, 118864.
  Karimi, Aghda Soheil; Holzapfel, Damian M.; Music, Denis; Unutulmazsoy, Yeliz; Mráz, Stanislav; Bogdanovski, Dimitri; Fidanboy, Gönenç; Hans, Marcus; Primetzhofer, Daniel; Méndez, Alba San José; Anders, André & Schneider, Jochen M.
  
• Modeling of very high frequency large-electrode capacitively coupled plasmas with a fully electromagnetic particle-in-cell code. Plasma Sources Science and Technology, 32(4), 044007.
  Eremin, D.; Kemaneci, E.; Matsukuma, M.; Mussenbrock, T. & Brinkmann, R. P.
  
• Physics-separating artificial neural networks for predicting initial stages of Al sputtering and thin film deposition in Ar plasma discharges. Journal of Physics D: Applied Physics, 56(8), 084003.
  Gergs, Tobias; Mussenbrock, Thomas & Trieschmann, Jan
  
• Thermodynamic quasi-equilibria in high power magnetron discharges: a generalized Poisson–Boltzmann relation. Plasma Sources Science and Technology, 32(5), 055012.
  Köhn, Kevin; Krüger, Dennis; Eremin, Denis; Xu, Liang & Brinkmann, Ralf Peter