Spectral diffusion arising from Si29 nuclear spin flip-flops, known to be a primary source of electron spin decoherence in silicon, is also predicted to limit the coherence times of neutral donor nuclear spins in silicon. Here, the impact of this mechanism on P31 nuclear spin coherence is measured as a function of Si29 concentration using X-band pulsed electron nuclear double resonance. The P31 nuclear spin echo decays show that decoherence is controlled by Si29 flip-flops resulting in both fast (exponential) and slow (nonexponential) spectral diffusion processes. The decay times span a range from 100 ms in crystals containing 50% Si29 to 3 s in crystals containing 1% Si29. These nuclear spin echo decay times for neutral donors are orders of magnitude longer than those reported for ionized donors in natural silicon. The electron spin of the neutral donors "protects" the donor nuclear spins by suppressing Si29 flip-flops within a "frozen core," as a result of the detuning of the Si29 spins caused by their hyperfine coupling to the electron spin.
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