Optimizing the Shape and Chemical Ordering of Nanoalloys with Specialized Walkers

Abstract

New algorithms for the optimization of alloy nanoparticles (nanoalloys) are presented. The new algorithms are based on the concept of multiple basin‐hopping walkers running in parallel, each with its own specialized task—the flying walker, exploring the energy landscape at high temperatures to sample different geometric structures, and the landing and hiking walkers mainly refining the optimization of chemical ordering at low temperatures. These algorithms are referred to as flying‐landing (FL) and flying‐landing‐hiking (FLH). The algorithms are tested against several benchmarks (AuCu and AuRh clusters of 400 atoms and PtNi clusters of 38 and 55 atoms). In all cases, both FL and FLH are shown to perform very well compared to previous results in the literature. In addition, the algorithms are applied to the optimization of larger AgCu nanoparticles, with sizes up to 4000 atoms, in order to establish the behavior of the mixing energy and to compare full global optimization of shape and chemical ordering with optimization of chemical ordering alone at a fixed shape. In general, the results show that the simultaneous optimization of shape and chemical ordering is necessary in many cases, and that the FLH approach is especially efficient for that purpose.

Tetrahedral Clusters Stabilized by Alloying

“…In this section, we describe the theoretical methods used. Global optimization searches were done by using our own basin-hopping code, , in which atomic interactions are approximated by the Gupta atomistic potential, which we describe in the following section. Density functional theory was used to estimate the energy of the structures found in the global optimization searches.…”

Understanding the shape effect on the structural, energetic, magnetic, and pressure properties of the 38 atom-Co-Fe-Pd nanoalloys using Gupta and DFT calculations

“…Recently, the most common shapes for face-centered cubic metal nanoalloys are truncated octahedra (TO), decahedra (Dh), and icosahedra (Ih), which have been the subject of intense research because they have unique properties [19]. The central goal of studying nanoalloys is to obtain detailed insight into their atomic structure and determine their configurations with the lowest potential energy [20]. Also, the focus has been on chemically ordered nanoalloys since many of the properties of metallic nanoalloys depend on the arrangement of their atoms, and accordingly, most of the studies available in the literature concentrate on obtaining the structures with the lowest energy at a given size [21].…”