The electric-quadrupole coupling constant of the ground states of the proton drip line nucleus 20Na(Iπ = 2+, T1/2 = 447.9 ms) and the neutron-deficient nucleus 21Na(Iπ = 3/2+, T1/2 = 22.49 s) in a hexagonal ZnO single crystal were precisely measured to be |eqQ/h| = 690 ± 12 kHz and 939 ± 14 kHz, respectively, using the multi-frequency β-ray detecting nuclear magnetic resonance technique under p...