Scalable construction of force-constant basis sets for large-scale anharmonic lattice-dynamical calculations

Abstract

A projector-based formulation of force constants in crystalline materials provides a systematic framework for constructing force-constant bases and determining force constants from force--displacement datasets while rigorously satisfying crystal symmetry, permutation symmetry, and translational invariance. In this work, we develop an efficient eigenvalue solver for projection matrices and integrate it into the projector-based framework. The proposed method substantially reduces the computational cost and enables practical calculations for large-scale systems, low-symmetry crystals, and higher-order force constants that are difficult to treat using conventional approaches. Applications to self-consistent phonon calculations for assessing the grain-boundary excess free energy, lattice thermal conductivity calculations in complex compounds, and fourth-order force-constant estimations demonstrate the efficiency and robustness of the proposed framework for large and complex materials systems.