Strongly anisotropic non-Kramers electron spin as a quantum coherence probe of angular fluctuations
Strongly anisotropic non-Kramers rare-earth ions combine giant longitudinal g-factors with a vanishing transverse component imposed by time-reversal symmetry, a combination that makes their spin transitions exquisitely sensitive to the orientation of the applied magnetic field. We show that this sensitivity carries a dual identity: it is simultaneously an overlooked decoherence channel and the basis for a spin-coherence-based angular probe. Using pulsed electron paramagnetic resonance at X-band, we report the first measurements of the quantum coherence of Tb$^{3+}$ in a native-doped CaWO$_4$ crystal (15 ppb) and map the Hahn-echo coherence time $T_2$ as a function of temperature (2 to 10 K) and resonant field ($10^3$ to $10^4$ G). A parameter-free model combining spin-lattice relaxation, instantaneous diffusion and spectral diffusion from all independently quantified impurities overestimates $T_2$ by an order of magnitude at low temperature and wrongly predicts the field dependence of $T_2$, inconsistent with the observed monotonic decrease of $T_2$ with $B_r$. A two-parameter extension, including dynamical angular fluctuations of the crystal axis, reproduces the full dataset across multiple setups and laboratories. Two controlled experiments nominally identical except for different mechanical configuration of the setup establish the mechanical origin of the dominant contribution. The two-parameter extension corresponds to an angular amplitude noise spectral density of overall order 36 n{\deg}/$\sqrt{Hz}$ from global external vibrations (ranging from 10 to 66 n{\deg}/$\sqrt{Hz}$ depending on the exact setup mechanical configuration) estimated at $\sim$ 2.5 kHz plus a temperature-dependent contribution assumed to come from local phonon-driven angular jitter. It identifies and highlights a decoherence pathway of practical relevance to any anisotropic solid-state spin system.