Searching for iron nanoparticles with a general-purpose Gaussian approximation potential

TL;DR

This paper introduces a versatile Gaussian approximation potential (GAP) model for iron, capable of accurately predicting properties of bulk structures, surfaces, and nanoparticles under various conditions, including Earth's core temperatures.

Contribution

The development of a comprehensive machine learning GAP model for iron that accurately describes diverse structures and conditions, extending stability predictions and nanoparticle configurations beyond previous limits.

Findings

GAP remains stable at Earth's core conditions.

Identified new low-energy iron nanoparticles with structures more stable than previous models.

Extended stable structure predictions up to 200 atoms, revealing disordered nanoparticle surfaces.

Abstract

We present a general-purpose machine learning Gaussian approximation potential (GAP) for iron that is applicable to all bulk crystal structures found experimentally under diverse thermodynamic conditions, as well as surfaces and nanoparticles (NPs). By studying its phase diagram, we show that our GAP remains stable at extreme conditions, including those found in the Earth's core. The new GAP is particularly accurate for the description of NPs. We use it to identify new low-energy NPs, whose stability is verified by performing density functional theory calculations on the GAP structures. Many of these NPs are lower in energy than those previously available in the literature up to $N_\text{atoms}=100$. We further extend the convex hull of available stable structures to $N_\text{atoms}=200$. For these NPs, we study characteristic surface atomic motifs using data clustering and low-dimensional embedding techniques. With a few exceptions, e.g., at magic numbers $N_\text{atoms}=59$, $65$, $76$ and $78$, we find that iron tends to form irregularly shaped NPs without a dominant surface character or characteristic atomic motif, and no reminiscence of crystalline features. We hypothesize that the observed disorder stems from an intricate balance and competition between the stable bulk motif formation, with bcc structure, and the stable surface motif formation, with fcc structure. We expect these results to improve our understanding of the fundamental properties and structure of low-dimensional forms of iron, and to facilitate future work in the field of iron-based catalysis.