Abstract
Throughout history, scientists and engineers have relied on the slow and serendipitous trial-and-error process for discovering and developing new materials. In contrast, an emerging theme in modern materials science is the notion of intelligent design of materials. Pioneered by the pharmaceutical industry and adapted for the purposes of materials science and engineering, the combinatorial approach represents a watershed in the process of accelerated discovery, development and optimization of materials. To survey large compositional landscapes rapidly, thousands of compositionally varying samples may be synthesized, processed and screened in a single experiment. Recent developments have been aided by innovative rapid characterization tools, and by advanced materials synthesis techniques such as laser molecular beam epitaxy which can be used to perform parallel-processed design and control of materials down to the atomic scale. Here we review the fast-growing field of combinatorial materials science, with an emphasis on inorganic functional materials.
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
Lebl, M. Parallel personal comments on 'classical' papers in combinatorial chemistry. J. Comb. Chem. 1, 3–24 (1999).
Takeuchi, I., Newsam, J.M., Wille, L.C., Koinuma, H. & Amis, E.J. (eds) Combinatorial and artificial intelligence methods in materials science. Mater. Res. Soc. Symp. Proc. 700 (2002).
Xiang, X.-D. & Takeuchi, I. (eds) Combinatorial Materials Synthesis (Dekker, New York, 2003).
Takeuchi, I., van Dover, R.B. & Koinuma, H. Combinatorial synthesis and evaluation of functional inorganic materials using thin-film techniques. Mater. Res. Soc. Bull. 27, 301–308 (2002).
Jandeleit, B., Turner, H.W., Uno, T., van der Beek, J.A.M. & Weinberg, W.H. CATTECH 2, 101 (1998).
Senken, S., Krantz, K., Ozturk, S., Zengin, V. & Onal, I. High-throughput testing of heterogeneous catalyst libraries using array microreactors and mass spectrometry. Angew. Chem. Int. Edn 38, 2794–2799 (1999).
Special issue on combinatorial research and high-throughput experimentation in polymer and materials research. Macromol. Rapid Commun. 24, (2003).
Xiang, X.-D. Combinatorial materials synthesis and screening: an integrated materials chip approach to discovery and optimization of functional materials. Annu. Rev. Mater. Sci. 29, 149–171 (1999).
Matsumoto, Y. et al. Combinatorial investigation of spintronic materials. Mater. Res. Soc. Bull. 28, 734–739 (2003).
Kennedy, K., Stefansky, T., Davy, G., Zacky, V.F. & Parker, E.R. Rapid mapping for determining ternary-alloy phase diagrams. J. Appl. Phys. 36, 3808–3810 (1965).
Miller, N.C. & Shirn, G.A. Co-sputtered Au–SiO2 cermet films. Appl. Phys. Lett. 10, 86–88 (1967).
Hanak, J.J., Gittleman, J.I., Pellicane, J.P. & Bozowski, S. The effect of grain size on the superconducting transition temperature of the transition metals. Phys. Lett. 30A, 201–202 (1969).
Hanak, J.J. The 'multi-sample concept' in materials research: synthesis, compositional analysis and testing of entire multicomponent systems. J. Mater. Sci. 5, 964–971 (1970).
Xiang, X.-D. et al. A combinatorial approach to materials discovery. Science 268, 1738–1740 (1995).
Koinuma, H. Quantum functional oxides and combinatorial chemistry. Solid State Ionics 108, 1–7 (1998).
Koinuma, H., Aiyer, N.H. & Matsumoto, Y. Combinatorial solid state materials science and technology. Sci. Technol. Adv. Mater. 1, 1–10 (2000).
Lippmaa, M., Kawasaki, M. & Koinuma, H. in Combinatorial Materials Synthesis (eds Xiang, X.-D. & Takeuchi, I.) Ch. 5 (Dekker, New York, 2003).
Wei, T., Xiang, X.-D., Wallace-Freedman, W.G. & Schultz, P.G. Scanning tip microwave near-field microscope. Appl. Phys. Lett. 68, 3506–3508 (1996).
Merrifield, R.B. Solid phase peptide synthesis. I. The synthesis of a tetrapeptide. J. Am. Chem. Soc. 85, 2149–2154 (1963).
Merrifield, R.B. Solid phase peptide synthesis. IV. The synthesis of methionyl-lysyl-bradykinin. J. Org. Chem. 29, 3100–3102 (1964).
Sato, K., Hibara, A., Tokeshi, M., Hisamoto, H. & Kitamori, T. Integration of chemical and biochemical analysis systems into a glass microchip. Anal. Sci. 19, 15–22 (2003).
Hanak, J.J. in Combinatorial Materials Synthesis (eds Xiang, X.-D. & Takeuchi, I, eds) 7–34 (Dekker, New York, 2003).
Koinuma, H., Nagata, H., Tsukahara, T., Gonda, S. & Yoshimoto, M. in Ext. Abstracts 22nd Conf. Solid State Devices and Materials (SSDM 90) 933–936 (Japanese Sociecty of Applied Physics, Tokyo, 1990).
Terashima, T. et al. Reflection high-energy electron diffraction oscillations during epitaxial growth of high-temperature superconducting oxides. Phys. Rev. Lett. 65, 2684–2687 (1990).
Kawasaki, M. et al. Atomic control of the SrTiO3 crystal surface. Science 266, 1540–1542 (1994).
Ohnishi, T. et al. Parallel integration and characterization of nanoscaled epitaxial lattices by concurrent molecular layer epitaxy and diffractometry. Appl. Phys. Lett. 79, 1282–1284 (2001).
Koida, T. et al. Temperature-gradient epitaxy under in situ growth mode diagnostics by scanning reflection high-energy electron diffraction. Appl. Phys. Lett. 80, 565–567 (2002).
Minami, H. et al. Rapid synthesis and scanning probe analysis of BaxSr1–xTiO3 composition spread films on a temperature gradient Si(100) substrate. Jpn J. Appl. Phys. 41, L149–L151 (2002).
Kubota, H. et al. Combinatorial synthesis and luminescent characteristics of RECa4O(BO3)3 epitaxial thin films. Appl. Surf. Sci. 223, 241–244 (2004).
Tamura, K. et al. Donor-acceptor luminescence in nitrogen-doped ScAlMgO4 (0001) substrates. Solid State Commun. 127, 265–269 (2003).
Fukumura, T. et al. Rapid construction of a phase diagram of doped Mott insulators with a composition-spread approach. Appl. Phys. Lett. 77, 3426–3428 (2000).
Hasegawa, K. et al. Amorphous stability of HfO2 based ternary and binary composition spread oxide films as alternative gate dielectrics. Appl. Surf. Sci. 223, 229–232 (2004).
Takahashi, R. et al. Design of combinatorial shadow masks for complete ternary-phase diagramming of solid state materials. J. Comb. Chem. 6, 50–53 (2004).
Matsumoto, Y. et al. Room-temperature ferromagnetism in transparent transition metal-doped titanium dioxide. Science 291, 854–856 (2001).
Takeuchi, I. et al. Identification of novel compositions of ferromagnetic shape memory alloys using composition spreads. Nature Mater. 2, 180–184 (2003).
Chang, H., Takeuchi, I. & Xiang, X.-D. A low-loss composition region identified from a thin-film composition spread of (Ba1–x–ySrxCay)TiO3 . Appl. Phys. Lett. 74, 1165–1167 (1999).
Chang, K.-S. et al. Multimode quantitative microwave microscopy of in situ grown epitaxial Ba1–xSrxTiO3 composition spreads. Appl. Phys. Lett. 79, 4411–4413 (2001).
Wang, J. et al. Identification of a blue photoluminescent composite material from a combinatorial library. Science 279, 1712–1714 (1998).
Semancik, S. & Cavicchi, R.E. Kinetically controlled chemical sensing using micromachined structures. Acc. Chem. Res. 31, 279–287 (1998).
Semancik, S. in Combinatorial Materials Synthesis (eds Xiang, X.-D. & Takeuchi, I.) Ch. 9 (Dekker, New York, 2003).
Potyrailo, R.A. & Morris, W.G. Multifunctional sensor system for high-throughput characterization of combinatorially developed materials. Rev. Sci. Instrum. 75, 2177–2186 (2004).
Potyrailo, R.A. & Morris, W.G. Parallel high-throughput microanalysis of materials using microfabricated full bridge device arrays. Appl. Phys. Lett. 84, 634–636 (2004).
Ohtani, M. et al. Concurrent X-ray diffractometer for high throughput structural diagnostics of epitaxial thin films. Appl. Phys. Lett. 79, 3594–3596 (2001).
Chang, W. in Combinatorial Materials Synthesis (eds Xiang, X.-D. & Takeuchi, I.) Ch. 10 (Dekker, New York, 2003).
Issacs, E.D. et al. Synchrotron X-ray microbeam diagnostics of combinatorial synthesis. Appl. Phys. Lett. 73, 1820–1822 (1998).
Chikyow, T. et al. A combinatorial approach in oxide/semiconductor interface research for future electronic devices. Appl. Surf. Sci. 189, 284–291 (2002).
van Dover, R.B., Schneemeyer, L.F. & Fleming, R.M. Discovery of a useful thin-film dielectric using a composition-spread approach. Nature 392, 162–164 (1998).
van Dover, R.B. & Schneemeyer, L.F. Deposition of uniform Zr–Sn–Ti–O films by on-axis reactive sputtering. IEEE Electron Device Lett. 19, 329–331 (1998).
Chang, H. et al. Combinatorial synthesis and high throughput evaluation of ferroelectric/dielectric thin film libraries for microwave applications. Appl. Phys. Lett. 72, 2185–2187 (1998).
Takeuchi, I. et al. Combinatorial synthesis and evaluation of epitaxial ferroelectric device libraries. Appl. Phys. Lett. 73, 894–896 (1998).
Chang, W. et al. The effect of (Ba,Sr) and (Mn,Fe,W) dopants of the microwave properties of (Ba,Sr)TiO3-based thin films. Mater. Res. Soc. Symp. Proc. 541, 699–704 (1999).
Chambers, S.A. & Farrow, R.F.C. New possibilities for ferromagnetic semiconductors. Mater. Res. Soc. Bull. 28, 729–733 (2003).
Tsui, F. et al. Novel germanium-based magnetic semiconductors. Phys. Rev. Lett. 91. 177203–1–4 (2003).
Shinde, S.R. et al. Co-occurrence of superparamagnetism and anomalous Hall effect in high reduced cobalt doped rutile TiO2–δ films. Phys. Rev. Lett. (in the press).
Sun, X.-D. & Xiang, X.-D. New phosphor (Gd2–xZnx)O3:Eu3+ with high luminescent efficiency and superior chromaticity. Appl. Phys. Lett. 72, 525–527 (1998).
Danielson, E. et al. A rare-earth phosphor containing one-dimensional chains through combinatorial methods. Science 279, 837–839 (1998).
Takeuchi, I. et al. Monolithic multichannel UV detector arrays and continuous phase evolution in MgxZn1–xO compositions spreads. J. Appl. Phys. 94, 7336–7340 (2003).
Yoo, Y.K. et al. Intermetallics 9, 541–545 (2001).
Itaka, K. et al. High-speed evaluation of thermoelectric materials using multi-channel measurement system. J. Thermal Anal. Calorimetry 69, 1051–1058 (2002).
Sun, T.X. & Jabbour, G.E. Combinatorial screening and optimization of luminescent materials and organic light-emitting devices. Mater. Res. Soc. Bull. 27, 309–315 (2002).
Yanase, I., Ohtaki, T. & Watanabe, M. Combinatorial study on nano-particle mixture prepared by robot system. Appl. Surf. Sci. 189, 292–299 (2002).
Kajiyama, A. et al. Synthesis and electrochemical properties of lithium chromium titanium oxide with Ramsdellite structure. J. Electrochem. Soc. 150, A157–A160 (2003).
Konishi, T. et al. Investigation of glass formation and color properties in the P2O5–TeO2–ZnO system. J. Non-Cryst. Solids 324, 58–66 (2003).
Meredith, J.C., Karim, A. & Amis, E.J. Combinatorial methods for investigations in polymer materials science. Mater. Res. Soc. Bull. 27, 330–336 (2002).
Special issue on combinatorial materials research and high-throughput experimentation in polymer and materials research. Macromol. Rapid Commun. 25, (2004).
Smotkin, E.S. & Diaz-Morales, R.R. New electrocatalysts by combinatorial methods. Annu. Rev. Mater. Res. 33, 557–579 (2003).
Senkan, S. Combinatorial heterogeneous catalysis: a new path in an old field. Angew. Chem. Int. Edn 40, 312–329 (2001).
Hendershot, R.J. et al. A novel reactor system for high throughput catalyst testing under realistic conditions. Appl. Catal. A 254, 107–120 (2003).
Rajan, K. in Combinatorial Materials Synthesis (eds Xiang, X.-D. & Takeuchi, I.) Ch. 13 (Dekker, New York, 2003).
Suh, C. & Rajan, K. Combinatorial design of semiconductor chemistry for bandgap engineering: 'virtual' combinatorial experimentation. Appl. Surf. Sci. 223, 148–158 (2004).
Huxtable, S., Cahill, D.G., Fauconnier, V., White, J.O. & Zhao, J.-C. Thermal conductivity imaging at micrometre-scale resolution for combinatorial studies of materials. Nature Mater. 3, 298–301 (2004).
Acknowledgements
We are grateful to many colleagues for collaboration and discussions over the years. We particularly thank the following colleagues for key contributions to some of this work (in alphabetical order): M. A. Aronova, L. A. Bendersky, H. Chang, K.-S. Chang, T. Chikyow, O. O. Famodu, T. Fukumura, C. Gao, T. Hasegawa, S. Inoue, K. Itaka, M. Kawasaki, L. Knauss, M. Lippmaa, S. E. Lofland, T. Makino, Y. Matsumoto, A. Miyamoto, M. Murakami, T. Ohnishi, A. Orozco, G. W. Rubloff, P. G. Schultz, Y. Segawa, S. Todoroki, R. D. Vispute, M. Watanabe, F. C. Wellstood, X.-D. Xiang, T. Yamamoto and Y. Yoo. H.K. acknowledges support from the CREST-JST 'Combinatorial molecular layer epitaxy' project (1996–2001) and the COMET project. I.T. acknowledges support from ONR N000140110761, N000140410085, NSF DMR0094265 (CAREER), NSF DMR 0231291 and NSF MRSEC DMR 00-80008.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing financial interests.
Rights and permissions
About this article
Cite this article
Koinuma, H., Takeuchi, I. Combinatorial solid-state chemistry of inorganic materials. Nature Mater 3, 429–438 (2004). https://doi.org/10.1038/nmat1157
Issue Date:
DOI: https://doi.org/10.1038/nmat1157
This article is cited by
-
Data-centric artificial olfactory system based on the eigengraph
Nature Communications (2024)
-
Combinatorial synthesis for AI-driven materials discovery
Nature Synthesis (2023)
-
Analysis of polycarbonate degradation at melt/FeCr-alloy interfaces as a function of the alloy composition by means of combinatorial thin film chemistry
SN Applied Sciences (2023)
-
Combinatorial synthesis of heteroepitaxial, multi-cation, thin-films via pulsed laser deposition coupled with in-situ, chemical and structural characterization
Scientific Reports (2022)
-
Machine learned synthesizability predictions aided by density functional theory
Communications Materials (2022)