Enlarging the quantum coherence times and gaining control over quantum effects in real systems are fundamental for developing quantum technologies. Molecular electron spin qubits are particularly promising candidates for realizing quantum information processing due to their modularity and tunability. Still, there is a constant search for tools to increase their quantum coherence times. Here we present how the mechanochemical introduction of active spin qubits in the form of 10% diluted copper(ii)-porphyrins in the diamagnetic PCN-223 and MOF-525 zirconium-MOF polymorph pair can be achieved. Furthermore, the encapsulation of fullerene during the MOF synthesis directs the process exclusively toward the rare PCN-223 framework with a controllable amount of fullerene in the framework channels. In addition to the templating role, the incorporation of fullerene increases the electron spin-lattice and phase-memory relaxation times, T1 and Tm. Besides decreasing the amount of nuclear spin-bearing solvent guests in the non-activated qubit frameworks, the observed improved relaxation times can be rationalized by modulating the phonon density of states upon fullerene encapsulation.
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