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In this paper we present fundamental studies elucidating the role of entropy in particle suspensions. We focus on systems composed of large colloidal particles along with a second, usually smaller species such as a particle or polymer. We describe direct measurements of these interactions in suspension, and we systematically show how these forces can be used to control the self-assembly of colloidal particles. The paper provides a unified review of the experiments from our laboratory, and in adoi:10.1098/rsta.2000.0809 fatcat:m2n4mznpwbe4rcbkxocadur5w4