Abstract
Our sol–gel transfer technique realizes highly crystalline metal oxide thin films on plastic substrates. In that technique a precursor gel film is fired at temperatures as high as 700 °C on an organic underlayer that is deposited beforehand on a single crystal silicon substrate. The resultant crystalline oxide film is transferred to a plastic substrate by heating the film on a hot plate and pressing a plastic substrate on it. The organic underlayer, which is completely lost during firing, critically facilitates the oxide film delamination from the silicon substrate. In order to answer the question how such a “lost” organic underlayer could be the key for the transfer, the effect of the underlayer thickness on the oxide film transferrability was investigated. Titania and zinc oxide precursor films were prepared by spin-coating on polyimide-polyvinylpyrrolidone and polyimide layers on Si(100) substrates, respectively, followed by firing and transfer to polycarbonate (PC) substrates. Quantitative evaluation based on image analysis demonstrated that thicker “lost” underlayers result in larger area fractions of the successfully transferred oxide films. Depth profile analyses by X-ray photoelectron spectroscopy excluded the residual carbon at the film/Si(100) interface as the delamination facilitator. On the other hand, atomic force microscopic observations demonstrated that thicker “lost” underlayers create larger surface roughness on both sides of the oxide films. It was concluded that such an increase in roughness decreased the contact area and brought the anchoring effect, reducing and increasing the film/Si(100) and film/PC adhesions, respectively, which facilitates the film transfer.
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R.H. Reuss, B.R. Chalamala, A. Moussessian, M.G. Kane, A. Kumar, D.C. Zhang, J.A. Rogers, M. Hatalis, D. Temple, G. Moddel, B.J. Eliasson, M.J. Estes, J. Kunze, E.S. Handy, E.S. Harmon, D.B. Salzman, J.M. Woodall, M.A. Alam, J.Y. Murthy, S.C. Jacobsen, M. Olivier, D. Markus, P.M. Campbell, E. Snow, Macroelectronics: perspectives on technology and applications. Proc. IEEE 93, 1239–1256 (2005). https://doi.org/10.1109/JPROC.2005.851237
Y. Sun, J.A. Rogers, Inorganic semiconductors for flexible electronics. Adv. Mater. 19, 1897–1916 (2007). https://doi.org/10.1002/adma.200602223
S. Sobajima, H. Okaniwa, N. Takagi, I. Sugiyama, K. Chiba, Production and properties of transparent electroconductive coating on polyester film. Jpn. J. Appl. Phys. 13, 475–478 (1974). https://doi.org/10.7567/JJAPS.2S1.475
K. Itoyama, Properties of Sn-doped indium oxide coatings deposited on polyester film by high rate reactive sputtering. J. Electrochem. Soc. 126, 691–694 (1979). https://doi.org/10.1149/1.2129111
R.P. Howson, J.N. Avaratsiotis, M.I. Ridge, C.A. Bishop, Properties of conducting transparent oxide films produced by ion plating onto room-temperature substrates. Appl. Phys. Lett. 35, 161–162 (1979). https://doi.org/10.1063/1.91065
A.W. Ott, R.P.H. Chang, Atomic layer-controlled growth of transparent conducting ZnO on plastic substrates. Mater. Chem. Phys. 58, 132–138 (1999). https://doi.org/10.1016/S0254-0584(98)00264-8
B.A. Latella, G. Triani, Z. Zhang, K.T. Short, J.R. Bartlett, M. Ignat, Enhanced adhesion of atomic layer deposited titania on polycarbonate substrates. Thin Solid Films 515, 3138–3145 (2007). https://doi.org/10.1016/j.tsf.2006.08.022
Y.C. Chen, C.F. Yang, E.Y. Hsueh, The application of AZOY transparent conductive oxide film in multifilm-coated polycarbonate optical glasses. J. Electrochem. Soc. 157, H987–H990 (2010). https://doi.org/10.1149/1.3474239
D. Kim, Deposition of indium tin oxide films on polycarbonate substrates by direct metal ion beam deposition, Appl. Surf. Sci. 218 (2003) 70–77, https://doi.org/10.1116/1.1605430
H. Kim, J.S. Horwitz, G.P. Kushto, Z.H. Kafafi, D.B. Chrisey, Indium tin oxide thin films grown on flexible plastic substrates by pulsed-laser deposition for organic light-emitting diodes. Appl. Phys. Lett. 79, 284–286 (2001). https://doi.org/10.1063/1.1383568
A. Miyake, T. Yamada, H. Makino, N. Yamamoto, T. Yamamoto, Properties of highly transparent conductive Ga-doped ZnO films prepared on polymer substrates by reactive plasma deposition with DC arc discharge. J. Photopolym. Sci. Technol. 22, 497–502 (2009). https://doi.org/10.2494/photopolymer.22.497
N. Al-Dahoudi, H. Bisht, C. Göbbert, T. Krajewski, M.A. Aegerter, Transparent conducting, anti-static and anti-static–anti-glare coatings on plastic substrates. Thin Solid Films 392, 299–304 (2001). https://doi.org/10.1016/S0040-6090(01)01047-1
K. Shimizu, H. Imai, H. Hirashima, K. Tsukuma, Low-temperature synthesis of anatase thin films on glass and organic substrates by direct deposition from aqueous solutions. Thin Solid Films 351, 220–224 (1999). https://doi.org/10.1016/S0040-6090(99)00084-X
M. Langlet, A. Kim, M. Audier, J.M. Herrmann, Sol–gel preparation of photocatalytic TiO2 films on polymer substrates. J. Sol–Gel Sci. Technol. 25, 223–234 (2002). https://doi.org/10.1023/A:1020259911650
A. Matsuda, T. Matoda, T. Kogure, K. Tadanaga, T. Minami, M. Tatsumisago, Formation of anatase nanocrystals-precipitated silica coatings on plastic substrates by the sol–gel process with hot water treatment. J. Sol–Gel Sci. Technol. 27, 61–69 (2003). https://doi.org/10.1023/A:1022632027151
N. Asakuma, T. Fukui, M. Toki, H. Imai, Low-temperature synthesis of ITO thin films using an ultraviolet laser for conductive coating on organic polymer substrates. J. Sol–Gel Sci. Technol. 27, 91–95 (2003). https://doi.org/10.1023/A:1022640228969
T. Königer, T. Rechtenwald, I. Al-Naimi, T. Frick, M. Schmidt, H. Münstedt, CO2-laser treatment of indium tin oxide nanoparticle coatings on flexible polyethyleneterephthalate substrates. J. Coat. Technol. Res. 7, 261–269 (2010). https://doi.org/10.1007/s11998-009-9181-5
H. Kozuka, Wet processing for the fabrication of ceramic thin films on plastics. J. Mater. Res. 28, 673–688 (2013). https://doi.org/10.1557/jmr.2013.13
H. Kozuka, H. Uchiyama, T. Fukui, M. Takahashi, Method to form ceramic films on plastic substrates, Japanese Patent 5924615 (2016)
H. Kozuka, T. Fukui, M. Takahashi, H. Uchiyama, S. Tsuboi, Ceramic thin films on plastics: a versatile transfer process for large area as well as patterned coating. ACS Appl. Mater. Interfaces 4, 6415–6120 (2012). https://doi.org/10.1021/am3019993
H. Kozuka, T. Fukui, H. Uchiyama, Sol–gel and transfer technique for fabricating dual ceramic thin film patterns on plastics. J. Sol–Gel Sci. Technol. 67, 414–419 (2013)
H. Kozuka, Sol–gel preparation of crystalline oxide thin films on plastics, in Handbook of Sol-Gel Science and Technology, 2nd edn, ed. by L.C. Klein, M. Aparicio, A. Jitianu (Springer, Basel, 2018), pp. 3271–3294. https://doi.org/10.1007/s10971-013-3081-y
Y. Qi, N.T. Jafferis, K. Lyons Jr., C.M. Lee, H. Ahmad, M.C. McAlpine, Piezoelectric ribbons printed onto rubber for flexible energy conversion. Nano Lett. 10, 524–528 (2010). https://doi.org/10.1021/nl903377u
K. Park, D.K. Lee, B.S. Kim, H. Jeon, N.E. Lee, D. Whang, H.J. Lee, Y.J. Kim, J.H. Ahn, Stretchable, transparent zinc oxide thin film transistors. Adv. Funct. Mater. 20, 3577–3582 (2010). https://doi.org/10.1002/adfm.201001107
K.I. Park, S. Xu, Y. Liu, G.T. Hwang, S.J.L. Kang, Z.L. Wang, K.J. Lee, Piezoelectric BaTiO3 thin film nanogenerator on plastic substrates. Nano Lett. 10, 4939–4943 (2010). https://doi.org/10.1021/nl102959k
H. Kozuka, M. Takahashi, K. Niinuma, H. Uchiyama, Fabrication of highly crystalline oxide thin films on plastics: Sol–gel transfer technique involving high temperature process. J. Asian Ceram. Soc. 4, 329–336 (2016). https://doi.org/10.1016/j.jascer.2016.06.003
N. Amano, M. Takahashi, H. Uchiyama, H. Kozuka, Transferability and adhesion of sol-gel-derived crystalline TiO2 thin films to different types of plastic substrates. Langmuir 33, 947–953 (2017). https://doi.org/10.1021/acs.langmuir.6b04142
T. Yamada, R. Okuda, H. Hirakoso, H. Kozuka, Sol–gel preparation of yttria-stabilized zirconia thin films and transfer to polycarbonate substrates. J. Sol–Gel Sci. Technol. 99, 554–561 (2019). https://doi.org/10.1007/s10971-019-05112-1
Y.M. Hunge, A.A. Yadav, V.L. Mathe, Oxidative degradation of phthalic acid using TiO2 photocatalyst. J. Mater. Sci. Mater. Electron. 29, 6183–6187 (2018). https://doi.org/10.1007/s10854-018-8593-3
J.G. Yu, X.J. Zhao, Q.N. Zhao, Effect of surface structure on photocatalytic activity of TiO2 thin films prepared by sol–gel method. Thin Solid Films 379, 7–14 (2000). https://doi.org/10.1016/S0040-6090(00)01542-X
Y.M. Hunge, A.A. Yadav, S.B. Kulkarni, V.L. Mathe, A multifunctional ZnO thin film based devices for photoelectrocatalytic degradation of terephthalic acid and CO2 gas sensing applications. Sensors Actuators B 274, 1–9 (2018). https://doi.org/10.1016/j.snb.2018.07.117
M. Ohyama, H. Kozuka, T. Yoko, Sol-gel preparation of ZnO films with extremely preferred orientation along (002) plane from zinc acetate solution. Thin Solid Films 306, 78–85 (1997). https://doi.org/10.1016/S0040-6090(97)00231-9
Y. Ohya, H. Saiki, T. Tanaka, Y. Takahashi, Microstructure of TiO2 and ZnO films fabricated by the sol–gel method. J. Am. Ceram. Soc. 79, 825–883 (1996). https://doi.org/10.1111/j.1151-2916.1996.tb08512.x|
M. Tahara, N.K. Cuong, Y. Nakashima, Improvement in adhesion of polyethylene by glow-discharge plasma. Surf. Coat. Technol. 173–174, 826–830 (2003). https://doi.org/10.1016/S0257-8972(03)00415-8
D. Sanchez-Rodriguez, J. Farjas, P. Roura, S. Ricart, N. Mestres, X. Obradors, T. Puig, Thermal analysis for low temperature synthesis of oxide thin films from chemical solutions. J. Phys. Chem. C 117, 20133–20138 (2013). https://doi.org/10.1021/jp4049742
B. Villarejo, C. Pop, S. Ricart, B. Mundet, A. Palau, P. Roura-Grabulosa, J. Farjas, T. Puig, X. Obradors, Pyrolysis study of solution-derived superconducting YBa2Cu3O7 films: disentangling the physico-chemical transformations. J. Mater. Chem. C 8, 10266–10282 (2020). https://doi.org/10.1039/d0tc01846e
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This research was financially supported by the Kazuchika Okura Memorial Foundation (45th Research Grant), and the Murata Science Foundation (31st Research Grant).
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Niinuma, K., Kozuka, H. Highly crystalline metal oxide thin films on plastic substrates prepared via firing and transfer: key role of the “lost” organic underlayer. J Mater Sci: Mater Electron 31, 18964–18979 (2020). https://doi.org/10.1007/s10854-020-04433-0
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DOI: https://doi.org/10.1007/s10854-020-04433-0