Site-fractions of indium impurity probe atoms occupying up to three inequivalent Al-sites in Al 3 Ti, Al 3 V and Al 3 Zr phases were measured using perturbed angular correlation of gamma rays (PAC). Sites were identified via characteristic nuclear quadrupole interactions. Ratios of site-fractions were measured in thermal equilibrium in the range 600 to 1,210 K. Arrhenius plots of the ratios were fitted with thermally activated expressions, yielding differences in vibrational entropies and siteenthalpies. Enthalpy differences were greatest for Al 3 Zr, ∼0.22 eV, and smaller for Al 3 Ti and Al 3 V, which is correlated with the excess volume of the transition-metal atom over the Al-atom. Vibrational entropy differences were small, in the range 0 to −0.25 k B .The site preference of dilute 111 In impurities in the Laves phase GdAl 2 was previously studied as a function of composition and temperature [1]. Occupied Gdand Al-sites were determined through measurements of quadrupole interactions using the method of perturbed angular correlation of gamma rays (PAC). In that study, 111 In impurity probe atoms were observed to switch between sites of different elements. The ratio of site fractions of indium solutes on Gd-and Al-sites was found to be thermally activated, with solutes transferring from the Gd-to Alsublattice with increasing temperature. Transfer takes place heuristically through the reaction In Gd + Al Al ⇔ In Al + Al Gd , in which Al Gd is an antisite atom that is either created or destroyed. Applying the law of mass action to the reaction leads to [In Al ][Al Gd ])/[In Gd ] = exp(−G tr /k B T), in which G tr is the free energy of transfer