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

Abstract

Graphdiyne, atomically-thin 2D carbon nanostructure based on sp-sp2 hybridization, is an appealing system potentially showing outstanding mechanical and optoelectronic properties. Surface-catalyzed coupling of halogenated sp-carbon-based molecular precursors represents a promising bottom-up strategy to fabricate extended 2D carbon systems with engineered structure on metallic substrates. Here, we investigate the atomic-scale structure and electronic and vibrational properties of an extended graphdiyne-like sp-sp2 carbon nanonetwork grown on Au(111) by means of on-surface synthesis. The formation of such 2D nanonetwork at its different stages as a function of the annealing temperature after the deposition is monitored by scanning tunneling microscopy (STM), Raman spectroscopy and combined with density functional theory (DFT) calculations. High-resolution STM imaging and the high sensitivity of Raman spectroscopy to the bond nature provide a unique strategy to unravel the atomic-scale properties of sp-sp2 carbon nanostructures. We show that hybridization between the 2D carbon nanonetwork and the underlying substrate states strongly affects its electronic and vibrational properties, modifying substantially the density of states and the Raman spectrum compared to the free standing system. This opens the way to the modulation of the electronic properties with significant prospects in future applications as active nanomaterials for catalysis, photoconversion and carbon-based nanoelectronics.

References in corpus (5)

• On-surface synthesis of graphene nanoribbons with zigzag edge topology
• Spatially Resolving Spin-split Edge States of Chiral Graphene Nanoribbons
• Short-Channel Field Effect Transistors with 9-Atom and 13-Atom wide Graphene Nanoribbons
• Effects of axial torsion on sp carbon atomic nanowires
• Raman and IR spectra of graphdiyne nanoribbons

Cited by in corpus (6)

• Topology-dependent conjugation effects in graphdiyne molecular fragments
• Graphdiynes interacting with metal surfaces: first-principles electronic and vibrational properties
• Electronic properties of two-dimensional rectangular graphyne based on phenyl-like building blocks
• Steric hindrance in the on-surface synthesis of diethynyl-linked anthracene polymers
• Vibrational properties of graphdiynes as 2D carbon materials beyond graphene
• Charge-Transfer Induced Reactivity in sp Carbon Atomic Wires: Towards 0-D sp-sp2 Nanostructures