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For binary fluid mixtures of spherical particles in which the two species aresufficiently different in size, the dominant wavelength of oscillations of thepair correlation functions is predicted to change from roughly the diameter ofthe large species to that of the small species along a sharp crossover line inthe phase diagram [C. Grodon, M. Dijkstra, R. Evans & R. Roth, J.Chem.Phys.121, 7869 (2004)]. Using particle-resolved colloid experiments in 3d wedemonstrate that crossover exists and that its location in the phase diagram isin quantitative agreement with the results of both theory and our Monte-Carlosimulations. In contrast with previous work [J. Baumgartl, R. Dullens, M.Dijkstra, R. Roth & C. Bechinger, Phys.Rev.Lett. 98, 198303 (2007)], where acorrespondence was drawn between crossover and percolation of both species, inour 3d study we find that structural crossover is unrelated to percolation.

Direct Observation in 3d of Structural Crossover in Binary Hard Sphere Mixtures