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Molecular vibrations play a key role in magnetic relaxation processes ofmolecular spin qubits as they couple to spin states, leading to the loss ofquantum information. Direct experimental determination of vibronic coupling iscrucial to understand and control the spin dynamics of these nano-objects,which represent the limit of miniaturization for quantum devices. Herein, wemeasure the vibrational properties of the molecular spin qubit$[$Ho(W$_5$O$_{18}$)$_2]^{9-}$ by means of magneto-infrared spectroscopy. Ourresults allow us to unravel the vibrational decoherence pathways in combinationwith $ab$ $initio$ calculations including vibronic coupling. We observefield-induced spectral changes near 63 and 370 cm$^{-1}$ that are modeled interms of $f$-manifold crystal field excitations activated by odd-symmetryvibrations. The overall extent of vibronic coupling in this system is limitedby a transparency window in the phonon density of states that acts to keep theintramolecular vibrations and $M_J$ levels apart. These findings advance theunderstanding of vibronic coupling in molecular magnets, place significantconstraints on the pattern of crystal field levels in these systems, andprovide a strategy for designing molecular spin qubits with improved coherencelifetimes.

Spectroscopic analysis of vibronic relaxation pathways in molecular spin qubit $[$Ho(W$_5$O$_{18}$)$_2]^{9-}$: sparse spectra are key