Fig. 4: Deterministic addressing the ¹³³Cs nuclear spin in the single crystal experiment.

A The single crystal Cr[Na] sample and the experiment set up that orients the B-field along the [001] crystallographic direction. The triangular surface of the crystal is the (111) surface. B Nuclear frequency analysis based on the three-pulse stimulated echo experiments (3P-ESEEM) performed on a Cr[Na] single crystal with the magnetic field (B) aligned close to the [001] direction selectively coupling to the ¹³³Cs nuclear spins. All nuclear frequencies associated with ¹³³Cs are identified through simulation fitting. The inset highlights the splitting of the peaks corresponding to four magnetically inequivalent Cs sites. This splitting arises from a slight misalignment of the B-field from the [001] direction, which also causes a minor reappearance of ^35,37Cl nuclear frequency peaks (the gray shaded area). See Fig. S5A–D, for further simulations clarifying this effect.