A straightforward way to determine the electric field gradient and principal axes frame (EFG-PAF) on single-crystal samples with spin-$\frac{3}{2}$ nuclei is demonstrated. Nuclear quadrupole resonance (NQR) spectroscopy is used to determine the Rabi frequency for ${}^{35}\mathrm{Cl}$ in a single crystal of potassium chlorate $\left({\mathrm{KClO}}_3\right)$ by comparing the NQR signal for powder and single-crystal samples. By exploiting the geometrical dependence of the Rabi frequency with respect to the excitation direction, EFG-PAF is readily determined. Furthermore, relaxation times $T_1$ and $T_2^{*}$ were measured at multiple temperatures ranging from 17 to $200\mathrm{K}$, extending the results of previous works to colder temperatures where new relaxation mechanisms become dominant. The experiments were performed in a cryogen-free cryostat, which posed distinct challenges compared to a conventional cryogenic cooling setup. The successful operation of the NQR probe within a cryogen-free cryostat has the potential to make the technique more accessible and widen applications.

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• Cryogenic technology
• Spin dynamics
• Spin relaxation
• Structural properties
• Crystalline systems
• Cryogenics
• Nuclear magnetic resonance
• Nuclear quadrupole resonance
• Radio frequency techniques
• Spectroscopy