| Sumario: | Metal–organic frameworks (MOFs) incorporating arrays of molecular spin qubits (quMOFs) offer a promising pathway toward scalable quantum computing. In this work, we introduce a novel quMOF, {[(Gd)3(mCB-L)4(NO3)(DMF)x]n·Solv}, constructed with a carborane linker and Gd(III) ions at three distinct coordination sites. We thoroughly characterize its magneto-thermal properties using dc/ac magnetometry, X-ray absorption spectroscopy, X-ray magnetic circular dichroism, and heat capacity measurements. The quantum computing potential is demonstrated through ab initio calculations and pulsed electron paramagnetic resonance on GdY-diluted analogues, revealing Tm= 0.7 μs and Rabi oscillations persisting up to 50 K. Each of the three isolated Gd(i) sites in GdY-MOFs functions as an 8-level qudit, accessible via X-band transitions. Notably, the triple-site Gd3 quMOF provides an unprecedented qudit with d = (2S + 1)3 = 512 states, capable of encoding up to 9 qubits, marking a significant advance in the scalability of molecular-based quantum computing.
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