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The covalent interaction of N-heterocyclic carbenes (NHCs) with transition metal atoms gives rise to distinctive frontier molecular orbitals (FMOs). These emergent electronic states have spurred the widespread adoption of NHC ligands in chemical catalysis and functional materials. Although formation of carbene-metal complexes in self-assembled monolayers on surfaces has been explored, design and electronic structure characterization of extended low-dimensional NHC-metal lattices remains elusive. Here we demonstrate a modular approach to engineering one-dimensional (1D) metal-organic chains and two-dimensional (2D) Kagome lattices using the FMOs of NHC–Au–NHC junctions to create low-dimensional molecular networks exhibiting intrinsic metallicity. Scanning tunneling spectroscopy and first-principles density functional theory reveal the contribution of C–Au–C π-bonding states to dispersive bands that imbue 1D- and 2D-NHC lattices with exceptionally small work functions. 

Graphene nanoribbons (GNRs), when synthesized with atomic precision by bottom–up chemical approaches, possess tunable electronic structure, and high theoretical mobility, conductivity, and heat dissipation capabilities, which makes them an excellent candidate for channel material in post-silicon transistors. Despite their immense potential, achieving highly transparent contacts for efficient charge transport—which requires proper contact selection and a deep understanding of the complex one-dimensional GNR channel-three-dimensional metal contact interface—remains a challenge. In this study, we investigated the impact of different electron-beam deposited contact metals—the commonly used palladium (Pd) and softer metal indium (In)—on the structural properties and field-effect transistor performance of semiconducting nine-atom wide armchair GNRs. The performance and integrity of the GNR channel material were studied by means of a comprehensive Raman spectroscopy analysis, scanning tunneling microscopy (STM) imaging, optical absorption calculations, and transport measurements. We found that, compared to Pd, In contacts facilitate favorable Ohmic-like transport because of the reduction of interface defects, while the edge structure quality of GNR channel plays a more dominant role in determining the overall device performance. Our study provides a blueprint for improving device performance through contact engineering and material quality enhancements in emerging GNR-based technology.