Local structural disorder in crystalline materials

Abstract

Local positional disorder in soft, anharmonic materials has emerged as a central factor in shaping their electronic, vibrational, optical, and transport properties. Viewed mainly as a source of performance degradation, recent theoretical insights reveal that local disorder profoundly influences the electronic structure and phonon dynamics, without inducing deep electronic traps or non-radiative recombination pathways. In this work, we highlight advances in modeling local disorder using polymorphous and anharmonic frameworks, showing how these methods explain experimental observations and predict new trends. We emphasize the role of disorder in the breakdown of the phonon quasiparticle picture and in modulating electron-phonon and phonon-phonon interactions, particularly in soft, anharmonic phases of matter, with significant effects on electrical and thermal transport. We outline opportunities for integrating these insights into predictive modeling for energy materials and propose combining advanced first-principles methods with machine learning.