Size, orientation, and boundary of graphene domains are the current focus of chemical vapor deposition (CVD) growth because they are closely related to graphene’s physical properties. Here, we study the domain structure of single-layer graphene grown by ambient pressure CVD over heteroepitaxial Cu(111) and Cu(100) films. Low energy electron microscope measurements reveal that the Cu(111) film gives uniform single-layer graphene whose orientation is consistent with the underlying Cu lattice for areas over 1 mm2. On the other hand, single-layer graphene grown on Cu(100) film exhibits clear multidomain structure with two main orientations rotated by 30°. Moreover, a weak Raman D-band is observed along the domain boundaries for the graphene grown on the Cu(100). Our results give new insights into the growth mechanism of CVD-grown graphene over Cu metals and offer a new direction for the realization of single-crystalline graphene.

Chiral materials possess left- and right-handed counterparts linked by mirror symmetry. These materials are useful for advanced applications in polarization optics, stereochemistry and spintronics. In particular, the realization of spatially uniform chiral films with atomic-scale control of their handedness could provide a powerful means for developing nanodevices with novel chiral properties. However, previous approaches based on natural or grown films, or arrays of fabricated building blocks, could not offer a direct means to program intrinsic chiral properties of the film on the atomic scale. Here, we report a chiral stacking approach, where two-dimensional materials are positioned layer-by-layer with precise control of the interlayer rotation (θ) and polarity, resulting in tunable chiral properties of the final stack. Using this method, we produce left- and right-handed bilayer graphene, that is, a two-atom-thick chiral film. The film displays one of the highest intrinsic ellipticity values (6.5 deg μm(-1)) ever reported, and a remarkably strong circular dichroism (CD) with the peak energy and sign tuned by θ and polarity. We show that these chiral properties originate from the large in-plane magnetic moment associated with the interlayer optical transition. Furthermore, we show that we can program the chiral properties of atomically thin films layer-by-layer by producing three-layer graphene films with structurally controlled CD spectra.

We report the scalable growth of aligned graphene and hexagonal boron nitride on commercial copper foils, where each film originates from multiple nucleations yet exhibits a single orientation. Thorough characterization of our graphene reveals uniform crystallographic and electronic structures on length scales ranging from nanometers to tens of centimeters. As we demonstrate with artificial twisted graphene bilayers, these inexpensive and versatile films are ideal building blocks for large-scale layered heterostructures with angle-tunable optoelectronic properties.

For electronic applications, synthesis of large-area, single-layer graphene with high crystallinity is required. One of the most promising and widely employed methods is chemical vapor deposition (CVD) using Cu foil/film as the catalyst. However, the CVD graphene is generally polycrystalline and contains a significant amount of domain boundaries that limit intrinsic physical properties of graphene. In this Perspective, we discuss the growth mechanism of graphene on a Cu catalyst and review recent development in the observation and control of the domain structure of graphene. We emphasize the importance of the growth condition and crystallinity of the Cu catalyst for the realization of large-area, single-crystalline graphene.

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Large hexagonal single-crystalline domains of single-layer graphene are epitaxially grown by ambient-pressure chemical vapor deposition over a thin Cu(111) film deposited on c-plane sapphire. The hexagonal graphene domains with a maximum size of 100 µm are oriented in the same direction due to the epitaxial growth. Reflecting high crystallinity, a clear band structure with the Dirac cone is observed by angle-resolved photoelectron spectroscopy (ARPES), and a high carrier mobility exceeding 4,000 cm2 V-1 s-1 is obtained on SiO2/Si at room temperature. Our epitaxial approach combined with large domain growth is expected to contribute to future electronic applications.

During the chemical vapor deposition (CVD) growth of graphene, graphene domains grown on a Cu surface merge together and form a uniform graphene sheet. For high-performance electronics and other applications, it is important to understand the interfacial structure of the merged domains, as well as their influence on the physical properties of graphene. We synthesized large hexagonal graphene domains with controlled orientations on a heteroepitaxial Cu film and studied the structure and properties of the interfaces between the domains mainly merged with the same angle. Although the merged domains have various interfaces with/without wrinkles and/or increased defect-related Raman D-band intensity, the intra-domain transport showed higher carrier mobility reaching 20,000 cm(2) V(-1) s(-1) on SiO2 at 280 K (the mean value was 7200 cm(2) V(-1) s(-1)) than that measured for inter-domain areas, 6400 cm(2) V(-1) s(-1) (mean value 2000 cm(2) V(-1) s(-1)). The temperature dependence of the mobility suggests that impurity scattering dominates at the interface even for the merged domains with the same orientation. This study highlights the importance of domain interfaces, especially on the carrier transport properties, in CVD-grown graphene.

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