Abstract

Graphene grown by high temperature molecular beam epitaxy on hexagonal boron nitride (hBN) forms continuous domains with dimensions of order 20 μm, and exhibits moiré patterns with large periodicities, up to ~30 nm, indicating that the layers are highly strained. Topological defects in the moiré patterns are observed and attributed to the relaxation of graphene islands which nucleate at different sites and subsequently coalesce. In addition, cracks are formed leading to strain relaxation, highly anisotropic strain fields, and abrupt boundaries between regions with different moiré periods. These cracks can also be formed by modification of the layers with a local probe resulting in the contraction and physical displacement of graphene layers. The Raman spectra of regions with a large moiré period reveal split and shifted G and 2D peaks confirming the presence of strain. Our work demonstrates a new approach to the growth of epitaxial graphene and a means of generating and modifying strain in graphene.

Highlights

  • The introduction of strain provides a route to modify both the electronic properties and phonon spectrum of graphene monolayers[1,2,3,4,5]

  • Attempts to grow graphene using molecular beam epitaxy (MBE), which might be expected to be well-suited to the growth of high-quality heterojunctions, on hBN31,32, as well as several other substrates including metal foils[33,34], SiC35 and sapphire[36,37,38], have so far not provided a route to the growth of large area epitaxial material

  • Carbon is evaporated by heating a high-purity graphite filament and the substrate temperature during growth is extremely high for MBE, we estimate ~1500 °C, much higher than the value reported in previous MBE studies of graphene growth

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Summary

Methods

We use a custom-designed dual-chamber GENxplor MBE system (base pressure ~10−10 Torr) supplied by Veeco which is modified to reach growth temperatures of 1850 °C and is compatible with substrates up to 3 inches in diameter. In this system the substrates are mounted in a vertical configuration with the substrate heater mounted above the substrate. The carbon deposition rate is estimated to be in the range 18–22 nm/hour from AFM measurements of the thickness of adsorbed carbon on the exposed sapphire regions of the substrate; note that the fraction of adsorbed carbon incorporated into epitaxial graphene on the adsorbed hBN flake is small, ~1%, so a growth time of ~4 hours is required to form a partial monolayer. CLS fitting to each spectrum in the map was performed using the Horiba Labspec 6 software

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