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TitleRelay-Like Exchange Mechanism through a Spin Radical between TbPc2 Molecules and Graphene/Ni(111) Substrates
Publication TypeJournal Article
Year of Publication2016
AuthorsMarocchi, S, Candini, A, Klar, D, Van den Heuvel, W, Huang, H, Troiani, F, Corradini, V, Biagi, R, De Renzi, V, Klyatskaya, S, Kummer, K, Brookes, NB, Ruben, M, Wende, H, del Pennino, U, Soncini, A, Affronte, M, Bellini, V
JournalACS Nano
Volume10
Pagination9353-9360
Abstract
We investigate the electronic and magnetic properties of TbPc2 single ion magnets adsorbed on a graphene/Ni(111) substrate, by density functional theory (DFT), ab initio complete active space self-consistent field calculations, and X-ray magnetic circular dichroism (XMCD) experiments. Despite the presence of the graphene decoupling layer, a sizable antiferromagnetic coupling between Tb and Ni is observed in the XMCD experiments. The molecule–surface interaction is rationalized by the DFT analysis and is found to follow a relay-like communication pathway, where the radical spin on the organic Pc ligands mediates the interaction between Tb ion and Ni substrate spins. A model Hamiltonian which explicitly takes into account the presence of the spin radical is then developed, and the different magnetic interactions at play are assessed by first-principle calculations and by comparing the calculated magnetization curves with XMCD data. The relay-like mechanism is at the heart of the process through which the spin information contained in the Tb ion is sensed and exploited in carbon-based molecular spintronics devices.
URLhttps://doi.org/10.1021/acsnano.6b04107
DOI10.1021/acsnano.6b04107
Library 
Soncini Group