Toward a theory of the third-order elastic modulus of crystals with A2 structure: The case of α-Fe

Abstract

The third-order elastic modulus of α-Fe were calculated based on the computation of lattice sums. The lattice sums were determined using an integer rational basis of invariants composed by vectors connecting equilibrium atomic positions in the crystal lattice. Irreducible interactions within clusters consisting of atomic pairs and triplets were taken into account in performing the calculations. Comparison with experimental data showed that the potential can be written in the form of $\varepsilon _9 = - \sum\nolimits_{i,k} {A_{19} r_{ik}^{ - 6} } + \sum\nolimits_{i,k} {A_{29} r_{ik}^{ - 12} + \sum\nolimits_{i,k,l} {Q_9 I_9^{ - 1} } }$, where $I_9 = \vec r_{ik}^2 \left[ {\left( {\vec r_{ik} \vec r_{kl} } \right)^2 + \left( {\vec r_{li} \vec r_{ik} } \right)^2 } \right] + \vec r_{kl}^2 \left[ {\left( {\vec r_{ik} \vec r_{kl} } \right)^2 + \left( {\vec r_{kl} \vec r_{li} } \right)^2 } \right] + \vec r_{li}^2 \left[ {\left( {\vec r_{li} \vec r_{ik} } \right)^2 + \left( {\vec r_{kl} \vec r_{li} } \right)^2 } \right]$. If the values of $\vec r_{ik}$ are scaled in half-lattice constant units, then $A_{19} = 1.22\left\lfloor {\tau ^9 } \right\rfloor GPa, A_{29} = 5.07 \times 10^2 \left\lfloor {\tau ^{15} } \right\rfloor GPa, Q_9 = 5.31\left\lfloor {\tau ^9 } \right\rfloor GPa$, and τ = 1.26 Å. It is shown that the condition of thermodynamic stability of a crystal requires that we allow for irreducible interactions in atom triplets in at least four coordination spheres. The analytical expressions for the lattice sums determining the contributions from irreducible interactions in the atom triplets to the second- and third-order elastic moduli of cubic crystals in the case of interactions determined by I ₉ are presented in the appendix.