<p>In this thesis we present a ⁷⁷Se NMR study of the iron selenide based high-temperature superconductor K_xFe_2−ySe₂ (T_c = 33 K). We observe NMR lineshapes as narrow as ∼ 4.5 kHz with an applied field along the crystal c-axis, and find no evidence for the co-existence of magnetic order with superconductivity. With an applied field along the ab plane, however, the lineshape splits into two peaks of equal intensities at all temperatures, suggesting that the tetragonal fourfold symmetry of the average structure may be locally lowered by vacancy superstructure. Knight shift data indicate that spin susceptibility decreases progressively with temperature, similar to other iron arsenide high-T_c systems. In the nuclear spin-lattice relaxation rate 1/T₁ we observe no Hebel-Slichter coherence peak, nor any enhancement in low frequency antiferromagnetic spin fluctuations in 1/T₁T. We also report on the effects of sulphur (S) substitution on the selenium sites in this system by conducting ⁷⁷Se NMR measurements on K_xFe_2−ySe_2−zS_z (z = 0.8, 1.6). We find that both spin susceptibility and low frequency spin fluctuations are suppressed with increasing S content along with T_c.</p> / Master of Science (MSc)