Evolutionary Search and Theoretical Study of Silicene Grain Boundaries' Mechanical Properties

Abstract

Defects such as grain boundaries (GBs) are almost inevitable during the synthesis process of 2D materials. To take advantage of the fascinating properties of 2D materials, understanding the nature and impact of various GB structures on the pristine 2D sheet is crucial. In this work, using an evolutionary algorithm search, we predict a wide variety of silicene GB structures with very different atomic structures compared to those found in graphene or hexagonal boron-nitride. Twenty-one GBs with the lowest energy were validated by density functional theory (DFT) - a majority of which were previously unreported to our best knowledge. Based on the diversity of the GB predictions, we found that the formation energy and mechanical properties can be dramatically altered by adatoms positions within a GB and certain types of atomic structures, such as four-atom rings. To study the mechanical behavior of these GBs, we apply strain to the GB structures stepwise and use DFT calculations to investigate the mechanical properties of 9 representative structures. It is observed that GB structures based on pentagon-heptagon pairs are likely to have similar or higher in-plane stiffness and strength compared with the zigzag orientation of pristine silicene. However, an adatom located at the hollow site of a heptagon ring can significantly deteriorate the mechanical strength. For all the structures, the in-plane stiffness and strength were found to decrease with increasing formation energy. For the failure behavior of GB structures, it was found that GB structures based on pentagon-heptagon pairs have failure behavior similar to graphene. We also found that the GB structures with atoms positioned outside of the 2D plane tend to experience phase transitions before failure. Utilizing the evolutionary algorithm, we locate diverse silicene GBs and obtain useful information for their mechanical properties.