Organic radicals are promising candidates for molecular spintronics due to their intrinsic magnetic moment, their low spin-orbit coupling, and their weak hyperfine interactions. Using a mechanically controlled break junction setup at both room and low temperatures (6 K), we analyze the difference in charge transport between two nitronyl nitroxide radicals (NNR): one with a backbone in the para configuration, the other with a backbone in the meta configuration. We find that para-NNR displays a Kondo resonance at 6 K, while meta-NNR does not. Additionally, the observed Kondo peak in the differential conductance has a roughly constant width independent of the conductance, consistent with a scenario where the molecule is coupled asymmetrically to the electrodes.

A promising approach to attain long-distance coherent spin propagation is accessing topological spin-polarized edge states in graphene. Achieving this without external magnetic fields necessitates engineering graphene band structure, obtainable through proximity effects in van der Waals heterostructures. In particular, proximity-induced staggered potentials and spin-orbit coupling are expected to form a topological bulk gap in graphene with gapless helical edge states that are robust against disorder. In this work, we detect the spin-polarized helical edge transport in graphene at zero external magnetic field, allowed by the proximity of an interlayer antiferromagnet, CrPS4. We show the coexistence of the quantum spin Hall (QSH) states and magnetism in graphene, where the induced spin-orbit and exchange couplings also give rise to a large anomalous Hall (AH) effect. The detection of the QSH states at zero external magnetic field, together with the AH signal that persists up to room temperature, opens the route for practical applications of magnetic graphene in quantum spintronic circuitries.

In this dissertation, we investigate charge transport in magnetic nano-objects. We use the mechanically-controlled break junction (MCBJ) technique to contact single molecules and use three different device geometries to optimize the process of contacting nanoparticles. We focus in particular on magnetic signatures in the quantum transport of these structures.