The optical conductivity of single layer graphene (SLG) can be significantly and reversibly modified when the Fermi level is tuned by electrical gating. However, so far this interesting property has rarely been applied to free-space two-dimensional (2D) photonic devices because the surface-incident absolute absorption of SLG is limited to 1%-2%. No significant change in either reflectance or transmittance would be observed even if SLG is made transparent upon gating. To achieve significantly enhanced surface-incident optical absorption in SLG in a device structure that also allows gating, here we embed SLG in an optical slot-antenna-coupled cavity (SAC) framework, simultaneously enhancing SLG absorption by up to 20 times and potentially enabling electrical gating of SLG as a step towards tunable 2D photonic surfaces. This framework synergistically integrates near-field enhancement induced by ultrahigh refractive index semimetal slot-antenna with broadband resonances in visible and infrared regimes, ~ 3 times more effective than a vertical cavity structure alone. An example of this framework consists of self-assembled, close-packed Sn nanodots separated by ~ 10 nm nanogaps on a SLG/SiO₂/Al stack, which dramatically increases SLG optical absorption to 10%-25% at λ = 600-1,900 nm. The enhanced SLG absorption spectrum can also be controlled by the insulator thickness. For example, SLG embedded in this framework with a 150 nm-thick SiO₂ insulating layer displays a distinctive red color in contrast to its surrounding regions without SLG on the same sample under white light illumination. This opens a potential path towards gate-tunable spectral reflectors. Overall, this work initiates a new approach towards tunable 2D photonic surfaces.

The metrology of two-dimensional (2D) materials such as graphene, boron nitride or molybdenum disulfide grown by chemical vapor deposition (CVD) is critical for the optimization of their synthesis. We demonstrate the use of film-induced frustrated etching (FIFE) as a facile, scalable method to reveal and quantify structural defects in continuous thin sheets. The sensitivity of the analysis technique to intentionally induced lattice defects in graphene compares favorably to the sensitivity of Raman spectroscopy. A strong correlation between the measured defectiveness and the maximum carrier mobility in graphene emphasizes the importance of the technique for growth optimization. Due to its ease and widespread availability, we anticipate that FIFE will find wide application in the characterization of CVD-synthesized 2D materials.

We report graphene films composed mostly of one or two layers of graphene grown by controlled carbon precipitation on the surface of polycrystalline Ni thin films during atmospheric chemical vapor deposition (CVD). Controlling both the methane concentration during CVD and the substrate cooling rate during graphene growth can significantly improve the thickness uniformity. As a result, one- or two-layer graphene regions occupy up to 87% of the film area. Single layer coverage accounts for 5%–11% of the overall film. These regions expand across multiple grain boundaries of the underlying polycrystalline Ni film. The number density of sites with multilayer graphene/graphite (> 2 layers) is reduced as the cooling rate decreases. These films can also be transferred to other substrates and their sizes are only limited by the sizes of the Ni film and the CVD chamber. Here, we demonstrate the formation of films as large as 1 in². These findings represent an important step towards the fabrication of large-scale high-quality graphene samples.