Structure and thermal fluctuation of one-dimensional AgO chains on Ag(110) surfaces studied with density functional theory and Monte Carlo simulations

Abstract

The structures of continuous and truncated AgO chains on Ag(110) surfaces are studied by using density functional theory (DFT) calculations and the thermal fluctuations of truncated chains are simulated by using the Monte Carlo method. Although it is known that oxygen elimination by CO from one-dimensional AgO chains takes place exclusively at chain ends when the chains keep a linear structure at low temperatures, the structure of chain ends has been unexplored. The DFT calculations reveal that oxygen-terminated chains are more stable than silver-terminated ones and have an enhanced density of states near the Fermi level at the terminal oxygen, which is consistent with scanning tunneling microscope (STM) observations. The Monte Carlo simulations with pairwise interactions between AgO units reproduce characteristic features observed in STM studies, including the existence of an onset temperature for the chain fluctuations and the oxygen-coverage dependence of average chain length. The onset temperature, on one hand, is largely controlled by attractive interactions in the direction parallel to chain growth. On the other hand, the spatial distribution of fragmented AgO chains depends strongly on repulsive interactions in the direction perpendicular to chains. In particular, the repulsive interactions ranging ten units of the lattice constant in the direction perpendicular to the AgO chains are essential to mimic STM observations, where fragmented chains almost keep the mutual distance inherent to the (nx1)-O phase even under thermal fluctuations.