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When single molecule magnets (SMMs) self-assemble into 2D networks on a surface, they interact via the π-electrons of their ligands. This interaction is relevant to the quantum entanglement between molecular qubits, a key issue in quantum computing. Here, we examine the role played by the unpaired radical electron in the top ligand of Tb double-decker SMMs by comparing the spectroscopic features of isolated and 2D assembled entities on surfaces. High-resolution scanning tunneling microscopy (STM) is used to evidence experimentally the Kondo resonance of the unpaired radical spins in clusters and islands and its quenching due to up-pairing at orbital overlaps. The presence or the absence of the Kondo feature in the dI/dV maps turns out to be a good measure of the lateral interaction between molecules in 2D networks. In a 2D cluster of molecules, the π-orbital lobes that are linked through the orbital overlap show paired-up electron wave function (one singly occupied molecular orbital (SOMO) with spin-up and the other with spin-down) and therefore do not experience the Kondo resonance in the experiment. As a result, small clusters built by STM-assisted manipulation of molecules show alternating Kondo features of quantum mechanical origin, from the monomer to the dimer and the trimer. On the other hand, when the TbPc 2 molecular clusters grow larger and form extended domains, a geometric rearrangement occurs, leading to the quenching of the Kondo signal on one lobe out of two. The even distribution of overlapping (SOMO) lobes on the perimeter of the molecule is induced by the square symmetry of the semi-infinite lattice and clearly distinguishes the lattice from the clusters.

Role of π-Radicals in the Spin Connectivity of Clusters and Networks of Tb Double-Decker Single Molecule Magnets