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It is known that the quantum-mechanical ground state of a nano-scale junctionhas a significant impact on its electrical transport properties. This becomesparticularly important in transistors consisting of a single molecule. Due tostrong electron-electron interactions and the possibility to access groundstates with high spins, these systems are eligible hosts of a current-blockadephenomenon called ground-state spin blockade. This effect arises from theinability of a charge carrier to account for the spin difference required toenter the junction, as that process would violate the spin selection rules.Here, we present a direct experimental demonstration of ground-state spinblockade in a high-spin single-molecule transistor. The measured transportcharacteristics of this device exhibit a complete suppression of resonanttransport due to a ground-state spin difference of 3/2 between subsequentcharge states. Strikingly, the blockade can be reversibly lifted by driving thesystem through a magnetic ground-state transition in one charge state, usingthe tunability offered by both magnetic and electric fields.

Ground-state spin blockade in a single-molecule junction