Abstract

<h2>Summary</h2> The extension of graphitic carbon nitride (g-CN) materials into optoelectronic applications beyond photocatalysis has long been anticipated due to their non-metallic composition, moderate electronic band gap, and excellent stability. However, large-scale synthesis of uniform two-dimensional (2D) g-CN films with high crystallinity and tunable thickness remains the bottleneck for their future applications in optoelectronic devices. Here, a vapor-phase transport-assisted condensation method has been developed for the wafer-scale synthesis of uniform 2D g-CN films with tunable thickness. First-principle calculations indicate the direct condensation from melem to heptazine-based carbon nitride enables the formation of high-quality g-CN films. A facile water-assisted transfer strategy is developed for subsequent fabrication on arbitrary substrate. A free-standing flexible photodetector array with strain-insensitive responsibility is demonstrated with the g-CN films as imaging pixels. This study provides a convenient route to wafer-scale growth of high-quality 2D g-CN films and paves the way to the g-CN-based electronic and optoelectronic devices.

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