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This article is licenced under a Creative Commons Attribution 3.0 Unported.-- et al.A metal-molecule-GNP assembly has been fabricated using an acetylene-terminated phenylene-ethynylene molecular monolayer, namely 4-((4-((4-ethynylphenyl)ethynyl)phenyl)ethynyl)benzoic acid (HOPEA), sandwiched between a gold substrate bottom electrode and gold nanoparticle (GNP) top contact electrode. In the first stage of the fabrication process, a monolayer of directionally oriented (carboxylate-to-gold) HOPEA was formed onto the bottom electrode using the Langmuir-Blodgett (LB) technique. In the second stage, the gold-substrate supported monolayer was incubated in a solution of gold nanoparticles (GNPs), which resulted in covalent attachment of the GNPs on top of the film via an alkynyl carbon-Au σ-bond thereby creating the metallic top electrode. Adsorption of the GNPs to the organic LB film was confirmed by both UV-vis absorption spectroscopy and X-ray photoemission spectroscopy (XPS), whilst the contact angle showed changes in the physical properties of the film surface as a result of top-coating of the LB film with the GNPs. Importantly, surface-enhanced Raman scattering (SERS) confirmed the covalent attachment of the metal particles to the LB film by formation of Au-C σ-bonds via a heterolytic cleavage of the alkyne C-H bond. Electrical properties of these nascent metal-molecule-GNP assemblies were determined from I-V curves recorded with a conductive-AFM in the Peak Force Tunneling AFM (PF-TUNA™) mode. The I-V curves obtained from these structures rule out the formation of any significant number of short-circuits due to GNP penetration through the monolayer, suggesting that this strategy of self-assembly of GNPs to alkyne-terminated monolayers is an effective 'soft' procedure for the fabrication of molecular junctions without damaging the organic layer. This journal is © the Partner Organisations 2014.P.C., I.G., F.P.-M., and S.M. are grateful for financial assistance from Ministerio de Economía y Competitividad from Spain and fondos FEDER in the framework of projects CTQ2012-33198, CSIC10-4E-805, and CSD2010-00024. P.C., F.P.-M. and S.M. are also grateful to the European SUDOE TRAIN2 project and the Nanolito network through the MAT2011-13099-E project funded by the Ministry of Economy of Spain for supporting this collaborative work. P.C., I.G. and S.M. acknowledge support from DGA and Fondos FEDER for funding Platon research group. H.M.O. and S.M. also thank their JIUZ-2013-CIE-05 grant. R.J.N., P.J.L. and S.M.-G. thank EPSRC for funding, and P.J.L. also gratefully acknowledges support from the Australian Research Council and the award of a Future Fellowship [FT120100073]. H.M.O. is grateful for financial assistance from Secretaría Nacional de Educación Superior, Ciencia, Tecnología e Innovación from Ministerio de Educación (Ecuador).Peer Reviewe

Preparation of nascent molecular electronic devices from gold nanoparticles and terminal alkyne functionalised monolayer films