Ultrafast Epitaxial Growth of Metre-Sized Single-Crystal Graphene on Industrial Cu Foil

TL;DR

This paper reports a rapid method to grow large, high-quality single-crystal graphene on industrial copper foil, enabling scalable production for advanced electronic applications.

Contribution

The authors developed an ultrafast, scalable process for epitaxial growth of metre-sized single-crystal graphene on industrial copper foil using a novel temperature-driven annealing technique.

Findings

Graphene film of 5 x 50 cm2 was grown in 20 minutes.

The graphene exhibited high mobility (~23,000 cm2V-1s-1) and low sheet resistance (~230 ohm/square).

The process produces high-quality, nearly misorientation-free single-crystal graphene.

Abstract

A foundation of the modern technology that uses single-crystal silicon has been the growth of high-quality single-crystal Si ingots with diameters up to 12 inches or larger. For many applications of graphene, large-area high-quality (ideally of single-crystal) material will be enabling. Since the first growth on copper foil a decade ago, inch-sized single-crystal graphene has been achieved. We present here the growth, in 20 minutes, of a graphene film of 5 x 50 cm2 dimension with > 99% ultra-highly oriented grains. This growth was achieved by: (i) synthesis of sub-metre-sized single-crystal Cu(111) foil as substrate; (ii) epitaxial growth of graphene islands on the Cu(111) surface; (iii) seamless merging of such graphene islands into a graphene film with high single crystallinity and (iv) the ultrafast growth of graphene film. These achievements were realized by a temperature-driven annealing technique to produce single-crystal Cu(111) from industrial polycrystalline Cu foil and the marvellous effects of a continuous oxygen supply from an adjacent oxide. The as-synthesized graphene film, with very few misoriented grains (if any), has a mobility up to ~ 23,000 cm2V-1s-1 at 4 K and room temperature sheet resistance of ~ 230 ohm/square. It is very likely that this approach can be scaled up to achieve exceptionally large and high-quality graphene films with single crystallinity, and thus realize various industrial-level applications at a low cost.