Edge-Energy-Driven Growth of Monolayer MnI₂ Islands on Ag(111): High-Resolution Imaging and Theoretical Analysis.

Abstract

The reduced dimensionality of thin transition metal dihalide films on single-crystal surfaces unlocks a diverse range of magnetic and electronic properties. However, achieving stoichiometric monolayer islands requires precise control over the growth conditions. In this study, we employ scanning probe microscopy to investigate the growth of MnI₂ on Ag(111) via single-crucible evaporation. The catalytic properties of the Ag(111) surface facilitate MnI₂ dehalogenation, leading to the formation of a reconstructed iodine adlayer that acts as a buffer layer for the growth of truncated hexagonal MnI₂ islands. These islands exhibit alternating edge lengths and distinct Kelvin potentials, as revealed by Kelvin probe force microscopy. Density functional theory (DFT) calculations support the experimentally observed island heights and lattice parameters and provide insights into the formation energies of both pristine and reconstructed edges. The asymmetry in edge lengths is attributed to differences in edge formation energies, driven by the position (up or down) of edge iodine atoms, as confirmed by DFT. This structural difference accounts for the observed variation in the Kelvin potential between the two types of island edge terminations.