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Progress in graphene-based single-molecule electronics

Five years ago we began to investigate the use of graphene nanoelectrodes for contacting individual molecules\,[1] and recently we began to translate this platform to a suspended TEM-compatible architecture. Graphene nanoelectrodes allow for non-covalent bonding of molecules\,[2], effective electrostatic gating, large-scale fabrication\,[3], atomic manipulation\,[4], and integration with other nano-electronic components\,[6]. The great success of this approach is only lessened by the fact that, unlike in the case of gold nanoelectrodes, graphene nanoelectrodes cannot simply be thought of as ideal, semi-infinite metal leads\,[6]. As the electronic and thermal properties of the graphene nanoelectrodes significantly influence the behaviour of the graphene-based single-molecule devices, the atomistic details of the graphene-molecule-graphene junction needs to be considered as a whole. Here, I will present a broad overview of the challenges and progress in understanding and controlling the interactions between individual molecules anchored to graphene nanoelectrodes and their environment and how these lessons can translate to emerging experiments manipulating atoms on the atomic scale in graphene and other 2D materials. I will focus on the influence of the unique material properties of graphene -- its two-dimensional nature, electronic band structure, and long mean-free path -- have on potential single-molecule device applications such as transistors\,[7], heat engines\,[5], and sensors\,[8].

[1] J.A. Mol, et al. , Nanoscale, 7, 13181 (2015)[2] C.S. Lau, et al., Phys. Chem. Chem. Phys., 16, 20398 (2014)[3] B. Limburg, et al., Adv. Funct. Mater. 1803629 (2018)[4] Dyck, Ondrej, et al., Appl. Phys. Lett., 111, 11 (2017)[5] P. Gehring, et al., Nano Lett., 17, 7055 (2017)[6] P. Gehring et al., ACS Nano, 11, 5325 (2017)[7] J.K. Sowa, et al., J. Chem. Phys. (in press, 2018)[8] P. Puczkarski, et al., ACS Nano, 12, 9451 (2018)