Abstract
The development of large-area, low-cost electronics for flat-panel displays, sensor arrays, and flexible circuitry depends heavily on high-throughput fabrication processes and a choice of materials with appropriate performance characteristics. For different applications, high charge carrier mobility, high electrical conductivity, large dielectric constants, mechanical flexibility or optical transparency may be required. Although thin films of metal oxides could potentially meet all of these needs, at present they are deposited using slow and equipment-intensive techniques such as sputtering. Recently, solution processing schemes with high throughput have been developed, but these require high annealing temperatures (Tanneal>400 °C), which are incompatible with flexible polymeric substrates. Here we report combustion processing as a new general route to solution growth of diverse electronic metal oxide films (In2O3, a-Zn–Sn–O, a-In–Zn–O, ITO) at temperatures as low as 200 °C. We show that this method can be implemented to fabricate high-performance, optically transparent transistors on flexible plastic substrates.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Mitzi, D. B. Solution Processing of Inorganic Materials (Wiley, 2009).
Reuss, R. H. et al. Macroelectronics: Perspectives on technology and applications. Proc. IEEE 93, 1239–1256 (2005).
Sun, Y. G. & Rogers, J. A. Inorganic semiconductors for flexible electronics. Adv. Mater. 19, 1897–1916 (2007).
Bae, S. et al. Roll-to-roll production of 30-inch graphene films for transparent electrodes. Nature Nanotech. 5, 574–578 (2010).
Ortiz, R. P., Facchetti, A. & Marks, T. J. High-k organic, inorganic, and hybrid dielectrics for low-voltage organic field-effect transistors. Chem. Rev. 110, 205–239 (2010).
Mannsfeld, S. C. B. et al. Highly sensitive flexible pressure sensors with microstructured rubber dielectric layers. Nature Mater. 9, 859–864 (2010).
Arias, A. C., MacKenzie, J. D., McCulloch, I., Rivnay, J. & Salleo, A. Materials and applications for large area electronics: Solution-based approaches. Chem. Rev. 110, 3–24 (2010).
Yan, H. et al. A high-mobility electron-transporting polymer for printed transistors. Nature 457, 679–686 (2009).
Naber, R. C. G. et al. High-performance solution-processed polymer ferroelectric field-effect transistors. Nature Mater. 4, 243–248 (2005).
Faber, H. et al. Low-temperature solution-processed memory transistors based on zinc oxide nanoparticles. Adv. Mater. 21, 3099–3104 (2009).
Rivnay, J. et al. Large modulation of carrier transport by grain-boundary molecular packing and microstructure in organic thin films. Nature Mater. 8, 952–958 (2009).
Sakanoue, T. & Sirringhaus, H. Band-like temperature dependence of mobility in a solution-processed organic semiconductor. Nature Mater. 9, 736–740 (2010).
Shimoda, T. et al. Solution-processed silicon films and transistors. Nature 440, 783–786 (2006).
van der Wilt, P. et al. Low-temperature polycrystalline silicon thin-film transistors and circuits on flexible substrates. MRS Bull. 31, 461–465 (2006).
Ju, S. Y. et al. Fabrication of fully transparent nanowire transistors for transparent and flexible electronics. Nature Nanotech. 2, 378–384 (2007).
Pal, B. N., Dhar, B. M., See, K. C. & Katz, H. E. Solution-deposited sodium beta-alumina gate dielectrics for low-voltage and transparent field-effect transistors. Nature Mater. 8, 898–903 (2009).
Cho, J. H. et al. Printable ion-gel gate dielectrics for low-voltage polymer thin-film transistors on plastic. Nature Mater. 7, 900–906 (2008).
Bong, H. et al. High-mobility low-temperature ZnO transistors with low-voltage operation. Appl. Phys. Lett. 96, 192115 (2010).
Alam, M. J. & Cameron, D. C. Investigation of annealing effects on sol–gel deposited indium tin oxide thin films in different atmospheres. Thin Solid Films 420, 76–82 (2002).
Wu, Y. L., Li, Y. N. & Ong, B. S. A simple and efficient approach to a printable silver conductor for printed electronics. J. Am. Chem. Soc. 129, 1862–1863 (2007).
Hu, L., Hecht, D. S. & Grüner, G. Carbon nanotube thin films: Fabrication, properties, and applications. Chem. Rev. 110, 5790–5844 (2010).
Nomura, K. et al. Room-temperature fabrication of transparent flexible thin-film transistors using amorphous oxide semiconductors. Nature 432, 488–492 (2004).
Nomura, K. et al. Thin-film transistor fabricated in single-crystalline transparent oxide semiconductor. Science 300, 1269–1272 (2003).
Wang, L. et al. High-performance transparent inorganic–organic hybrid thin-film n-type transistors. Nature Mater. 5, 893–900 (2006).
Lee, C. G. & Dodabalapur, A. Solution-processed zinc–tin oxide thin-film transistors with low interfacial trap density and improved performance. Appl. Phys. Lett. 96, 243501 (2010).
Choi, C. G., Seo, S. J. & Bae, B. S. Solution-processed indium-zinc oxide transparent thin-film transistors. Electrochem. Solid-State Lett. 11, H7–H9 (2008).
Kim, H. S., Byrne, P. D., Facchetti, A. & Marks, T. J. High performance solution-processed indium oxide thin-film transistors. J. Am. Chem. Soc. 130, 12580–12581 (2008).
Lee, D. H., Chang, Y. J., Herman, G. S. & Chang, C. H. A general route to printable high-mobility transparent amorphous oxide semiconductors. Adv. Mater. 19, 843–847 (2007).
Ong, B. S., Li, C. S., Li, Y. N., Wu, Y. L. & Loutfy, R. Stable, solution-processed, high-mobility ZnO thin-film transistors. J. Am. Chem. Soc. 129, 2750–2751 (2007).
Seo, S. J., Choi, C. G., Hwang, Y. H. & Bae, B. S. High performance solution-processed amorphous zinc tin oxide thin film transistor. J. Phys. D 42, 035106 (2009).
MacDonald, W. A. Engineered films for display technologies. J. Mater. Chem. 14, 4–10 (2004).
Jeong, S., Ha, Y. G., Moon, J., Facchetti, A. & Marks, T. J. Role of gallium doping in dramatically lowering amorphous-oxide processing temperatures for solution-derived indium zinc oxide thin-film transistors. Adv. Mater. 22, 1346–1350 (2010).
Kim, H. S. et al. Low-temperature solution-processed amorphous indium tin oxide field-effect transistors. J. Am. Chem. Soc. 131, 10826–10827 (2009).
Aksu, Y. & Driess, M. A low-temperature molecular approach to highly conductive tin-rich indium tin oxide thin films with durable electro-optical performance. Angew. Chem. Int. Ed. 48, 7778–7782 (2009).
Meyers, S. T. et al. Aqueous inorganic inks for low-temperature fabrication of ZnO TFTs. J. Am. Chem. Soc. 130, 17603–17609 (2008).
Hoffmann, R. C., Differ, S., Issanin, A. & Schneider, J. J. Solution processed ZnO—challenges in processing and performance on flexible substrates. Phys. Status Solidi A 207, 1590–1595 (2010).
Asakuma, N., Fukui, T., Toki, M. & Imai, H. 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).
Merzhanov, A. G. The chemistry of self-propagating high-temperature synthesis. J. Mater. Chem. 14, 1779–1786 (2004).
Tukhtaev, R. K. et al. Metal sulfide synthesis by self-propagating combustion of sulphur-containing complexes. Inorg. Mater. 38, 985–991 (2002).
Yi, H. C. & Moore, J. J. Self-propagating high-temperature (combustion) synthesis (SHS) of powder-compacted materials. J. Mater. Sci. 25, 1159–1168 (1990).
Epifani, M., Melissano, E., Pace, G. & Schioppa, M. Precursors for the combustion synthesis of metal oxides from the sol–gel processing of metal complexes. J. Eur. Ceram. Soc. 27, 115–123 (2007).
Sato, T. Preparation and thermal decomposition of indium hydroxide. J. Therm. Anal. Calorim. 82, 775–782 (2005).
Pramanik, N. C., Das, S. & Kumar Biswas, P. The effect of Sn(IV) on transformation of co-precipitated hydrated In(III) and Sn(IV) hydroxides to indium tin oxide (ITO) powder. Mater. Lett. 56, 671–679 (2002).
Donley, C. et al. Characterization of indium–tin oxide interfaces using X-ray photoelectron spectroscopy and redox processes of a chemisorbed probe molecule: Effect of surface pretreatment conditions. Langmuir 18, 450–457 (2002).
Kamiya, T., Nomura, K. & Hosono, H. Origins of high mobility and low operation voltage of amorphous oxide TFTs: Electronic structure, electron transport, defects and doping. J. Display Technol. 5, 273–288 (2009).
Hosono, H., Nomura, K., Ogo, Y., Uruga, T. & Kamiya, T. Factors controlling electron transport properties in transparent amorphous oxide semiconductors. J. Non-Cryst. Solids 354, 2796–2800 (2008).
Ip, K. et al. Contacts to ZnO. J. Cryst. Growth 287, 149–156 (2006).
Cui, Y., Zhong, Z. H., Wang, D. L., Wang, W. U. & Lieber, C. M. High performance silicon nanowire field effect transistors. Nano Lett. 3, 149–152 (2003).
Addison, C. C. & Simpson, W. B. Tin(IV) nitrate: the relation between structure and reactivity of metal nitrates. J. Chem. Soc. 598–602 (1965).
Donaldson, J.D. & Moser, W. Basic tin(II) nitrate. J. Chem. Soc. 1996–2000 (1961).
Greve, D. W. Field Effect Devices and Application: Devices for Portable, Low-Power, and Imaging Systems (Prentice-Hall, 1988).
Acknowledgements
The research was supported by the MRSEC program of NSF (DMR-0520513) at the Northwestern University Materials Research Center and by AFOSR (FA9550-08-1-0331). Microscopy and XPS studies were performed in the EPIC, NIFTI, KECK-II facilities of NUANCE Center at Northwestern University. NUANCE Center is supported by NSF-NSEC, NSF-MRSEC, Keck Foundation, the State of Illinois, and Northwestern University.
Author information
Authors and Affiliations
Contributions
M-G. Kim, M. G. Kanatzidis, A.F. and T.J.M. designed the research. M-G. Kim carried out the experiments. M-G. Kim, M. G. Kanatzidis, A.F. and T.J.M. analysed the data and co-wrote the manuscript.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing financial interests.
Supplementary information
Rights and permissions
About this article
Cite this article
Kim, MG., Kanatzidis, M., Facchetti, A. et al. Low-temperature fabrication of high-performance metal oxide thin-film electronics via combustion processing. Nature Mater 10, 382–388 (2011). https://doi.org/10.1038/nmat3011
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/nmat3011
This article is cited by
-
Pulse irradiation synthesis of metal chalcogenides on flexible substrates for enhanced photothermoelectric performance
Nature Communications (2024)
-
High-speed hybrid complementary ring oscillators based on solution-processed organic and amorphous metal oxide semiconductors
Communications Materials (2023)
-
Enabling low-drift flexible perovskite photodetectors by electrical modulation for wearable health monitoring and weak light imaging
Nature Communications (2023)
-
Two quasi-interfacial p-n junctions observed by a dual-irradiation system in perovskite solar cells
npj Flexible Electronics (2023)
-
Ammonia gas detection by solution combustion-processed pristine & Ti-doped ZnO transparent films: a reverse effect of doping on gas response
Journal of Materials Science: Materials in Electronics (2023)