Origin of Reduced Coercive Field in ScAlN: Synergy of Structural Softening and Dynamic Atomic Correlations

TL;DR

This study reveals that the reduced coercive field in ScAlN ferroelectrics results from combined structural softening and dynamic atomic correlations, uncovered through advanced simulations at near-first-principles accuracy.

Contribution

It introduces a machine-learning-based simulation framework to elucidate the atomic-scale mechanisms behind Ec reduction in ScAlN, integrating structural and dynamic effects.

Findings

Dynamic atomic displacements trigger polarization reversal.

Sc atoms exhibit larger thermal vibrations influencing switching.

Cooperative atomic rearrangements lower the switching barrier.

Abstract

Among wurtzite-type ferroelectrics, scandium-doped aluminum nitride (ScAlN) has emerged as a leading candidate for CMOS-compatible low-voltage memory, combining strong spontaneous polarization with process compatibility. A remarkable feature of this system is the pronounced reduction of the coercive field (Ec) with increasing Sc concentration; however, its microscopic origin remains poorly understood at the atomic scale, particularly under finite temperature and applied electric fields. Here, we integrate a density-functional-theory-accurate machine-learning force field with an equivariant neural-network-based Born effective charge model to perform large-scale electric-field-driven molecular dynamics simulations at near-first-principles accuracy. The framework correctly reproduces the experimentally observed qualitative trends in key experimental trends, including the decrease in the c/a ratio and the monotonic reduction of Ec with increasing Sc content. Beyond static structural softening, we uncover a dynamic mechanism underlying Ec reduction. Sc atoms exhibit larger thermal vibrations and undergo preceding displacements during switching, acting as dynamic triggers for polarization reversal. Moreover, the displacement correlation between Sc and Al atoms evolves systematically with composition, enhancing cooperative atomic rearrangements and lowering the effective switching barrier. These results demonstrate that Ec reduction in ScAlN arises from the synergy of structural softening and dynamic correlation evolution, providing a new perspective for designing hexagonal ferroelectrics.