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Artificial magnetic molecules are suitable hosts to one or several spinqubits, which could then implement small-scale algorithms. In order to becomeof practical use, such molecular spin processors need to increase the dimension$d$ of the available computational space and fulfill the highly demandingconditions that warrant universal operations. Here, we design, synthesize andfully characterize dissymetric molecular dimers hosting either one or twoGd(III) ions. The strong sensitivity of Gd(III) magnetic anisotropy to thesymmetry of its local coordination gives rise to different zero-fieldsplittings at each coordination site. As a result, the [LaGd] and [GdLu]complexes provide realizations of distinct $d = 8$ spin qudits, whereas the[Gd$_{2}$] dimer meets all requirements, including a complete set ofoperations, to act as a $d = 64$ all-electron spin qudit (or, equivalenty, assix addressable qubits). Electron paramagnetic resonance experiments show thatthe relevant resonant transitions between different spin states can becoherently controlled, with coherence times T$_{M}$ of the order of $1$ $\mu$slimited by intramolecular hyperfine interactions. Coordination complexes withembedded quantum functionalities are promising building blocks for quantumcomputation and simulation hybrid platforms.

A dissymmetric [Gd$_{2}$] coordination molecular dimer hosting six addressable spin qubits