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Graphdiyne, atomically-thin 2D carbon nanostructure based on sp-sp2hybridization, is an appealing system potentially showing outstandingmechanical and optoelectronic properties. Surface-catalyzed coupling ofhalogenated sp-carbon-based molecular precursors represents a promisingbottom-up strategy to fabricate extended 2D carbon systems with engineeredstructure on metallic substrates. Here, we investigate the atomic-scalestructure and electronic and vibrational properties of an extendedgraphdiyne-like sp-sp2 carbon nanonetwork grown on Au(111) by means ofon-surface synthesis. The formation of such 2D nanonetwork at its differentstages as a function of the annealing temperature after the deposition ismonitored by scanning tunneling microscopy (STM), Raman spectroscopy andcombined with density functional theory (DFT) calculations. High-resolution STMimaging and the high sensitivity of Raman spectroscopy to the bond natureprovide a unique strategy to unravel the atomic-scale properties of sp-sp2carbon nanostructures. We show that hybridization between the 2D carbonnanonetwork and the underlying substrate states strongly affects its electronicand vibrational properties, modifying substantially the density of states andthe Raman spectrum compared to the free standing system. This opens the way tothe modulation of the electronic properties with significant prospects infuture applications as active nanomaterials for catalysis, photoconversion andcarbon-based nanoelectronics.

acs applied nano materials

Structural, Electronic, and Vibrational Properties of 2D Graphdiyne-Like  Carbon Nanonetwork Synthesized on Au(111): Implications for the Engineering  of sp-sp2 Carbon Nanostructures