Pauli blockade mechanisms -- whereby carrier transport through quantum dots (QDs) is blocked due to selection rules even when energetically allowed -- are of both fundamental and technological interest, as a direct manifestation of the Pauli exclusion principle and as a key mechanism for manipulating and reading out spin qubits. Pauli spin blockade is well established for systems such as GaAs QDs, where the two-electron spin-singlet ground state is separated from the three triplet states higher in energy. However, Pauli blockade physics remains largely unexplored for systems in which the Hilbert space is expanded due to additional degrees of freedom, such as the valley quantum numbers in carbon-based materials or silicon. Here we report experiments on coupled graphene double QDs in which the spin and valley states can be precisely controlled. We demonstrate that gate and magnetic-field tuning allows switching between a spin-triplet--valley-singlet ground state with charge occupancy (2,0), where valley-blockade is observed, and a spin-singlet--valley-triplet ground state, where spin blockade is shown. These results demonstrate how the complex two-particle Hilbert space of graphene quantum dots can be unravelled experimentally, with implications for future spin and valley qubits.
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