Fermi Level Engineering and Mechanical Properties of High Entropy Carbides (2101.04885v1)

Abstract: Fermi level engineering and mechanical properties evolution in high entropy carbides are investigated by theoretical and experimental means. Massive elemental diversity in high entropy ceramics broadens the compositional space but imposes great challenges in composition selection and property investigation. We have utilized the valence electron concentration (VEC) descriptor to design and predict properties of high entropy carbides. The VEC regulates the Fermi energy and systematically alters the bonding characteristics of materials. As a result, mechanical properties evolve as function of the VEC. At VEC 8.4, the strong {\sigma} bonding states stem from filled overlapping metal d and carbon p orbitals, which results in maximum resistance to shear deformation and highest hardness. Beyond or below the optimum VEC point of 8.4, mechanical response degrades due to filling or emptying of energy orbitals that facilitates shear deformation. Furthermore, the optimum VEC point can shift based on the constituent metals that formulate the high entropy carbide. Our analyses demonstrate strong correlation between calculated hardness and shear modulus. As an experimental complement, a set of high entropy carbides are synthesized, and mechanical properties investigated. The measured hardness follows theoretical predictions and the highest hardness of ~30 GPa is achieved at VEC 8.4. In contrast, hardness decreases by 50% when VEC is 9.4. Designing high entropy carbides based on VEC and understanding mechanical properties at an electronic level enables one to manipulate the composition spectrum to procure a desired mechanical response from a chemically disordered crystal.