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Prediction and accelerated laboratory discovery of previously unknown 18-electron ABX compounds

Nature Chemistry volume 7, pages 308–316 (2015)Cite this article

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Abstract

Chemists and material scientists have often focused on the properties of previously reported compounds, but neglect numerous unreported but chemically plausible compounds that could have interesting properties. For example, the 18-valence electron ABX family of compounds features examples of topological insulators, thermoelectrics and piezoelectrics, but only 83 out of 483 of these possible compounds have been made. Using first-principles thermodynamics we examined the theoretical stability of the 400 unreported members and predict that 54 should be stable. Of those previously unreported ‘missing’ materials now predicted to be stable, 15 were grown in this study; X-ray studies agreed with the predicted crystal structure in all 15 cases. Among the predicted and characterized properties of the missing compounds are potential transparent conductors, thermoelectric materials and topological semimetals. This integrated process—prediction of functionality in unreported compounds followed by laboratory synthesis and characterization—could be a route to the systematic discovery of hitherto missing, realizable functional materials.

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Figure 1: N–X–(8−N) compounds obtained by the insertion of a group X element (Ni, Pd, Pt) into an eight-valence electron lattice.
Figure 2: (N+1)–IX–(8−N) compounds obtained by the insertion of a group IX element (Co, Rh, Ir) into a nine-valence electron lattice.
Figure 3: The 18-electron ABX compounds predicted by theory and synthesized in this work.
Figure 4: Discovery of the HfIrSb ternary material.
Figure 5: Electronic structure of 18-electron ABX in the cubic LiAlSi-type structure ().

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Acknowledgements

This work was performed at Northwestern University and the University of Colorado Boulder with funding provided by the US Department of Energy, Office of Science, Basic Energy Sciences, and Energy Frontier Research Centers, under Contract No. DE- AC36-08GO28308 to the National Renewable Energy Laboratory. We thank G. Trimarchi for helpful discussions.

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  1. Romain Gautier and Xiuwen Zhang: These authors contributed equally to this work

Authors and Affiliations

  1. Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, 60628-3113, Illinois, USA

    Romain Gautier, Linhua Hu, Yuyuan Lin, Tor O. L. Sunde, Danbee Chon & Kenneth R. Poeppelmeier

  2. University of Colorado, Boulder, 80309, Colorado, USA

    Xiuwen Zhang, Liping Yu & Alex Zunger

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Contributions

X.Z. performed the stability calculations as well as property calculations other than the phonon and dielectric constants carried out by L.Y. R.G., Y.L., L.H., T.O.L.S. and D.C. performed the synthesis and characterization of new ABX materials. The experimental work was supervised by K.R.P. Furthermore, X.Z., R.G. and L.Y. contributed to the writing of the paper. K.R.P. and A.Z. directed the analysis of the results and writing of the paper.

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Correspondence to Kenneth R. Poeppelmeier or Alex Zunger.

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Gautier, R., Zhang, X., Hu, L. et al. Prediction and accelerated laboratory discovery of previously unknown 18-electron ABX compounds. Nature Chem 7, 308–316 (2015). https://doi.org/10.1038/nchem.2207

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