AbstractThe quadrupole coupling constant, eQVzz/h, for 111Cd probe nuclei in CdxMg1−x, alloys (x = 0.0 to 1.0) is measured as a function of temperature and composition, using the time differential perturbed angular correlation technique. The observed temperature dependence of the electric field gradient (EFG), Vzz can be described by a T3/2‐relation for each of the compositions studied, except in the cases where phase transformations take place. From the measured concentration dependence of the EFG in the disordered h.c.p. phase of the alloy with lattice constants c and a, plots for the variation of a3(eQVzz/h) with c/a are made at different temperatures. These experimental results are discussed, using a theory of the EFG in metals, which predicts such a plot to belinear.