IntroductionColloidal crystals are the subject of intense research for several reasons. First, owing to their speci®c length and time scales their properties are readily accessible by various forms of light scattering and microscopy. Second, a number of interesting questions of fundamental interest in condensed matter physics can be addressed in a well-de®ned model systems. This concerns both equilibrium properties (like diusive dynamics, structure or phase behaviour), response to external ®elds (like electrokinetic properties or sedimentation) and situations far from equilibrium (like the glass transition, shear-melting or crystallisation kinetics). Third, however, important applications may also result from a better understanding of the generic properties. Optical-band-gap materials are one of these.Recently focus has shifted from single-component suspensions to mixtures. The most prominent examples deal with hard-sphere or hard-sphere-polymer mixtures of large size dierence, where phase separation is observed owing to attractive terms in the potential of the mean force [1,2]. Much less is known about charged mixtures. Only a few reports exist on the phase behaviour [3,4,5], and fewer on even other properties, like shear rigidity [6], diusion [7,8] or crystallisation kinetics.We report on a mixture of two species of polystyrene latex spheres in deionised aqueous suspension. Their size ratio is C 0.85. Such a small value should not induce an entropically driven instability. Nevertheless, the phase behaviour is not immediately obvious. The formation of alloy structures of glasses or of precipitats can be expected. Alloys may either be compositionally ordered (e.g. of NaCl structure) or disordered (e.g. Cu/Au). We conducted a number of dierent experiments to comprehensively characterise the resulting solids. Besides the static structure factor, S(q), we also measured the conductivity, r, and the static shear modulus, G. The former is very sensitive to the formation of precipitates; the latter has been shown to yield valuable information about the local crystal structure [9]. Finally, we also report some of the ®rst dynamic light scattering measurements on polycrystalline samples. Their interpretation can be qualitative only, since a rigorous scattering theory of such nonergodic and inhomogeneous materials is still demanded. The combination of our results shows that at low-to-intermediate particle concentrations randomly substituted alloys of body-centered-cubic (bcc) structure are formed.Abstract We prepared colloidal crystals from aqueous suspensions of spherical, charged polystyrene spheres under deionised conditions. Using a home-built multipurpose light scattering apparatus we measured the static structure factor, the static shear modulus and the intermediate scattering function. In addition we also monitored also the conductivity as a function of the composition and the particle number density. For the mixture investigated the data are well described assuming the formation of randomly substituted body-centere...