The PDF file includes:

• Note S1. Derivation of the nonsecular Redfield equations
• Note S2. Lattice parameters and spin Hamiltonian
• Note S3. K points and phonon’s line width convergence
• Note S4. Number of spins convergence
• Note S5. Effect of numerical noise
• Table S1. Lattice parameters for the VO(acac)₂ molecular crystal.
• Table S2. Spin Hamiltonian parameters for VO(acac)₂.
• Fig. S1. Spin relaxation time as function of external fields for different values of k points.
• Fig. S2. Spin relaxation time as function of the Gaussian breadth for different external fields.
• Fig. S3. Spin relaxation time as function of the number of coupled spins.
• Fig. S4. Effect of numerical noise on spin relaxation time.
• Reference (32)

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Other Supplementary Material for this manuscript includes the following:

• Spin-phonon coupling coefficients and ab initio calculations� input files.