Revealing low-energy surfaces of multinary compounds by controlling surface coordination environments
Abstract
When modeling surfaces of multinary compounds, conventional cleavage planes often cut through strongly bonded polyhedra, resulting in unphysical surface energies. Here, we introduce SALAMI (Symmetric Atomic Layers for Arbitrary Multinary Interfaces), a Python package that generates symmetric, charge-neutral, dipole-free, and low-energy slab models for multinary compounds. SALAMI performs combinatorial searches to selectively remove surface atoms and generate corrugated terminations that preserve optimal coordination environments. We applied this workflow to all symmetrically inequivalent crystallographic orientations with Miller indices up to 2 for two prototypical structures: the solid-state electrolyte Li3PS4 and the transparent conducting oxide ZnSb2O6. Density functional theory calculations reveal that Li3PS4 must preserve all PS4 units to achieve the minimum surface energy. For ZnSb2O6, low-energy surfaces are achieved by partial undercoordination of surface Sb atoms to SbO5 or SbO4 from the bulk SbO6, depending on the surface orientations. Compared to surface models generated with unconstrained coordination, applying constraints to achieve optimal local coordination environments significantly lowers surface energies, shrinking the volume of the predicted Wulff shape by approximately 20%. Our results demonstrate that meticulous control of local coordination environments is necessary for accurately predicting the surface energetics of multinary compounds.
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BibTeX
@misc{xie2026revealing,
title = {{Revealing low-energy surfaces of multinary compounds by controlling surface coordination environments}},
author = {Weihang Xie and Harshan Reddy Gopidi and Zhengyu Liu and Romain Claes and Alexander G. Squires and Keith T. Butler and David O. Scanlon and Pieremanuele Canepa},
howpublished = {arXiv},
year = {2026},
month = aug,
doi = {10.48550/arxiv.2608.28903},
eprint = {2608.28903},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2608.28903},
}
RIS
TY - UNPB
TI - Revealing low-energy surfaces of multinary compounds by controlling surface coordination environments
AU - Weihang Xie
AU - Harshan Reddy Gopidi
AU - Zhengyu Liu
AU - Romain Claes
AU - Alexander G. Squires
AU - Keith T. Butler
AU - David O. Scanlon
AU - Pieremanuele Canepa
PY - 2026
DA - 2026/08/28
PB - arXiv
DO - 10.48550/arxiv.2608.28903
UR - https://arxiv.org/abs/2608.28903
AB - When modeling surfaces of multinary compounds, conventional cleavage planes often cut through strongly bonded polyhedra, resulting in unphysical surface energies. Here, we introduce SALAMI (Symmetric Atomic Layers for Arbitrary Multinary Interfaces), a Python package that generates symmetric, charge-neutral, dipole-free, and low-energy slab models for multinary compounds. SALAMI performs combinatorial searches to selectively remove surface atoms and generate corrugated terminations that preserve optimal coordination environments. We applied this workflow to all symmetrically inequivalent crystallographic orientations with Miller indices up to 2 for two prototypical structures: the solid-state electrolyte Li3PS4 and the transparent conducting oxide ZnSb2O6. Density functional theory calculations reveal that Li3PS4 must preserve all PS4 units to achieve the minimum surface energy. For ZnSb2O6, low-energy surfaces are achieved by partial undercoordination of surface Sb atoms to SbO5 or SbO4 from the bulk SbO6, depending on the surface orientations. Compared to surface models generated with unconstrained coordination, applying constraints to achieve optimal local coordination environments significantly lowers surface energies, shrinking the volume of the predicted Wulff shape by approximately 20%. Our results demonstrate that meticulous control of local coordination environments is necessary for accurately predicting the surface energetics of multinary compounds.
ER -