High-Throughput Screening of the Thermoelastic Properties of Ultrahigh-Temperature Ceramics

Abstract

Ultrahigh-temperature ceramics (UHTCs) are a group of materials with high technological interest because of their applications in extreme environments. However, their characterization at high temperatures represents the main obstacle for their fast development. Obstacles are found from an experimental point of view, where only few laboratories around the world have the resources to test these materials under extreme conditions, and also from a theoretical point of view, where actual methods are expensive and difficult to apply to large sets of materials. Here, a new theoretical high-throughput framework for the prediction of the thermoelastic properties of materials is introduced. This approach can be systematically applied to any kind of crystalline material, drastically reducing the computational cost of previous methodologies up to 80% approximately. This new approach combines Taylor expansion and density functional theory calculations to predict the vibrational free energy of any arbitrary strained configuration, which represents the bottleneck in other methods. Using this framework, elastic constants for UHTCs have been calculated in a wide range of temperatures with excellent agreement with experimental values, when available. Using the elastic constants as the starting point, other mechanical properties such a bulk modulus, shear modulus, or Poisson ratio have been also explored, including upper and lower limits for polycrystalline materials. Finally, this work goes beyond the isotropic mechanical properties and represents one of the most comprehensive and exhaustive studies of some of the most important UHTCs, charting their anisotropy and thermal and thermodynamical properties.

Advances in data‐assisted high‐throughput computations for material design

“…They found that high pressure could enhance the resistance to volume, elastic, and shear deformations of XTiO 3 ceramics. Nath et al [248] . developed an HTC framework for predicting the thermoelastic properties of materials, which combines Taylor expansion and DFT calculations to predict the vibrational free energies of arbitrarily strained structures.…”

Ab initio thermo-elasticity of δ-MHx (M=Zr, Ti)

“…Owing to the much increased computational effort required for such modelling, only relatively few efforts have been directed towards computing temperature dependent elastic constants. They have mostly been limited to FCC [39][40][41], HCP [40,42,43], diamond [44] and body-centred cubic crystals [45,46], while only few works have addressed more complex ceramics [47,48]. But to the best of the author's knowledge, no efforts have been directed towards elucidating the thermal dependence of the elastic constants of hydrides.…”

First‐principles study of the thermal properties of Zr2C and Zr2CO

“…High‐throughput materials screening methods are able to identify candidate compositions with desirable properties without time‐consuming trial‐and‐error experimental studies 13–16 . Such methods are especially valuable for investigating the properties of ultra‐high‐temperature ceramics due to the difficulties in testing materials under extreme conditions 17 . For example, atomistic simulations were used to predict the thermal conductivities of ZrC x ceramics with carbon stoichiometries ranging from x = 0.9 to 1 18 .…”

“…[13][14][15][16] Such methods are especially valuable for investigating the properties of ultra-high-temperature ceramics due to the difficulties in testing materials under extreme conditions. 17 For example, atomistic simulations were used to predict the thermal conductivities of ZrC x ceramics with carbon stoichiometries ranging from x = 0.9 to 1. 18 The thermal conductivities were predicted to increase with increasing temperature as had been observed in experimental studies.…”