Free Standing Epitaxial Oxides Through Remote Epitaxy: The Role of the Evolving Graphene Microstructure

TL;DR

This study investigates how the microstructure of graphene affects the quality of remote epitaxial oxide films, demonstrating that larger graphene grains reduce damage and improve film crystallinity, enabling scalable exfoliation and transfer.

Contribution

It reveals the direct link between graphene microstructure and epitaxial oxide quality, introducing a controlled aperture method to minimize graphene damage during growth.

Findings

Larger graphene grains (>300 microns) result in less damage and higher quality oxide films.

Bi-layer graphene with large grains enables exfoliation and transfer of 4 mm x 5 mm oxide layers.

Damage is more pronounced at graphene grain boundaries than within grains.

Abstract

Remote epitaxy has garnered considerable attention as a promising method that facilitates the growth of thin films that replicate the crystallographic characteristics of a substrate by utilizing two-dimensional (2D) material interlayers like graphene. The resulting film can be exfoliated to form a freestanding membrane, and the substrate, if expensive, can be reused. However, atomically thin 2-D materials are susceptible to damage before and during film growth in the chamber, leading to a poor epitaxy. Oxide remote epitaxy using graphene, the most commonly available 2D material, is particularly challenging because the conventional conditions employed for the growth of epitaxial oxides also degrade graphene. In this study, we show for the first time that a direct correlation exists between the microstructure of graphene, its getting defective on exposure to the pulsed laser deposition plume, and the crystalline quality of the barium titanate film deposited on top. A controlled aperture method was used to reduce graphene damage. Even so, the degree of damage is more at the graphene grain boundaries than within the grains. Large grain-sized greater than 300 microns, graphene suffered less damage and yielded a film comparable to that grown directly on a strontium titanate substrate with a rocking curve half width of 0.6 degrees. Using large grain-sized bi-layer graphene, 4 mm x 5 mm oxide layers were successfully exfoliated and transferred onto SiOx-Si. These insights pave the way for the heterogeneous integration of functional oxides on foreign substrates, holding significant implications for commercializing perovskite oxides by integrating them with Si-CMOS and flexible electronics.