High-throughput search for transparent conducting oxydes

Academic Partners : Profs Geoffroy Hautier and Xavier Gonze

Funding : European Union

Grant Agreement : PC1G11-GA-2012-321988

Period : 1 August 2012 - 31 July 2015

Summary

Transparent conducting oxides (TCO) show the rare combination of high electronic conductivity (10-3 to 10-4 Ohm.cm) and transparency in the visible range. TCO materials are critical in many industrial applications. Their importance in energy related applications (e.g., in low-emissivity windows and thin-film photovoltaics) make them of special interest for “green technologies”. On the longer term, the development of new TCOs could also enable entirely new technologies such as transparent electronics.
While there is a great need for finding new TCOs, the purely experimental search can be very time consuming as the chemical space to explore is very large, and one would have to synthesize and characterize each possible new materials candidate. Fortunately, researchers have nowadays access to a very powerful tool called ab initio computations. The ab initio techniques rely on the basic laws of physics to compute properties of materials (sometimes even before they have even been synthesized). An emerging approach is to use these ab initio techniques on a very large scale to perform so-called high-throughput computations. The idea is very simple yet powerful.

By computing properties for thousands of different materials we can right away select the most promising ones and guide experiments towards them. Luckily, many of the properties of importance for TCOs can be nowadays computationally assessed (e.g. transparency, carrier mobilities and concentrations).

This project aims at performing the first high-throughput computational search for new TCOs.
There are two kinds of TCOs: the n-type (with electrons as carriers) and the p-type (with the absence of electrons, or holes, as carriers). While the n-type TCOs are largely commercialized and show good performances, the few known p-type TCOs show very poor quality. Unfortunately, the lack of a good p-type TCO impedes the development of many critical future technologies (e.g., transparent electronics or better solar cells). Our high-throughput infrastructure has already identified several novel potential p-type TCOs that had never been considered as TCO before. From a database of more than 4,000 known oxides only a handful satisfied the criteria to be a good p-type TCO. This illustrates how powerful high-throughput computational can be in solving the “needle in a haystack” problem of new materials discovery. Experimentalists can now use our results to focus on those promising chemistries identified through computing. This approach saves an enormous amount of time. Our work goes even further. Not only have we identified the most promising oxides but the generated data has been used to discover the design rules to make very high conductivity p-type TCOs. For instance, materials containing a certain type of chemical element (tin 2+) are especially prone to form very good p-type TCOs. Those new chemical recipe will certainly give a new impulse to the quest for high performance p-type TCOs.

Publications :

H. Zhu, G. Hautier, U. Aydemir, Z. M. Gibbs, G. Li, S. Bajaj, J.-H. Pöhls, D. Broberg, W. Chen, A. Jain, M. A. White, M. Asta, G. J. Snyder, K. Persson, G. Ceder, Computational and experimental investigation of TmAgTe2 and XYZ2 compounds, a new group of thermoelectric materials identified by first- principles high-throughput screening, Journal of Materials Chemistry C, 2015

A. Jain, S. P. Ong, W. Chen, M. Bharat, X. Qu, M. Kocher, M. Brafman, G. Petretto, G.-M. Rignanese, G. Hautier, D. Gunter, K. A. Persson FireWorks: a dynamic workflow system designed for high-throughput applications, Concurrency and Computation: Practice and Experience, 22, 6, 2015

D. Bilc, G. Hautier, D. Waroquiers, G.-M. Rignanese, P. Ghosez, Large thermoelectric power factors in bulk semiconductors by band engineering of highly-directional electronic states, Physical Review Letters, 114, 136601, 2015

A. Bathia, G. Hautier, T. Nilgianskul, A. Miglio, G.-M. Rignanese, X. Gonze, J. Suntivich, High-Mobility Bismuth-based Transparent P-Type Oxide from High-throughput Material Screening, 2015, submitted http://arxiv.org/abs/1412.4429

G. Hautier, A. Miglio, D. Waroquiers, G.-M. Rignanese, X. Gonze, How does chemistry influence electron effective mass in oxides? A high-throughput computational analysis, Chemistry of Materials, 26, 5447, 2014

A. Miglio, R.Saniz, D. Waroquiers, M. Stankovski, M. Giantomassi, G. Hautier, G.-M. Rignanese, X. Gonze, Computed electronic and optical properties of SnO2 under compressive stress, Optical Materials, 38, 161, 2014

J. B. Varley, V. Lordi, A. Miglio, G. Hautier, Electronic structure and defect properties of B 6 O from hybrid functional and many-body perturbation theory calculations : A possible ambipolar transparent conductor. Physical Review B - Condensed Matter and Materials Physics, 90, 045205, 2014

G. Hautier, A. Miglio, G. Ceder, G.-M. Rignanese, X. Gonze, Identification and design principles of low hole effective mass p-type transparent conducting oxides. Nature Communications, 4, 2292, 2013

S. P. Ong, W.D. Richards, A. Jain, G. Hautier, M. Kocher, S. Cholia, D. Gunter, V.L. Chevrier, K.A. Persson, G. Ceder, Python Materials Genomics (pymatgen): A robust, open-source python library for materials analysis. Computational Materials Science, 68, 314–319, 2013

A. Jain, S.P. Ong, G. Hautier, W. Chen, W. D. Richards, S. Dacek, S. Cholias, D. Gunter, D. Skinner, G. Ceder, K. A. Persson, Commentary: The Materials Project: A materials genome approach to accelerating materials innovation. APL Materials, 1(1), 011002, 2013