doi:10.1021/acsami.5c06002engBartolomé, ElenaLi, Xiao-BaoArauzo, AnaLuzón, JavierGarcía-Rubio, InésPlanas, José GinerA Triple-Site Gd3 Carborane Metal–Organic Framework toward Scalable Quantum ComputingART-2025-144500Metal–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.2025http://zaguan.unizar.es/record/16188710.1021/acsami.5c06002http://zaguan.unizar.es/record/161887oai:zaguan.unizar.es:161887info:eu-repo/grantAgreement/ES/AEI/CEX2023-001263-Sinfo:eu-repo/grantAgreement/ES/DGA/E09-23Rinfo:eu-repo/grantAgreement/ES/DGA/E12-23Rinfo:eu-repo/grantAgreement/ES/MICINN/PID2021-127287NB-I00info:eu-repo/grantAgreement/ES/MICINN/PID2022-136892NB-I00info:eu-repo/grantAgreement/ES/MICINN/PID2022-138492NB-I00info:eu-repo/grantAgreement/ES/MICIU/CEX2023-001286-Sinfo:eu-repo/grantAgreement/ES/MICIU/PRTR-C17.I1ACS applied materials & interfaces (2025), [14 pp.]byhttps://creativecommons.org/licenses/by/4.0/deed.esinfo:eu-repo/semantics/openAccess