We present pulsed electron-nuclear double resonance (ENDOR) experiments which enable us to characterize the coupling between bismuth donor spin qubits in Si and the surrounding spin bath of 29Si impurities which provides the dominant decoherence mech
anism (nuclear spin diffusion) at low temperatures (< 16 K). Decoupling from the spin bath is predicted and cluster correlation expansion simulations show near-complete suppression of spin diffusion, at optimal working points. The suppression takes the form of sharply peaked divergences of the spin diffusion coherence time, in contrast with previously identified broader regions of insensitivity to classical fluctuations. ENDOR data suggest that anisotropic contributions are comparatively weak, so the form of the divergences is largely independent of crystal orientation.
