This paper describes a study of the generation and flow of photocurrent through junctions containing three-dimensional arrays of colloidal CdSe quantum dots (QDs) of either a single size or multiple sizes. The electrodes were indium tin oxide (ITO) covered with a thin layer of poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS) and a eutectic alloy of Ga and In (EGaln). We measured the current-voltage characteristics of the junctions in the dark and under illumination, with various sources and wavelengths of excitation, and their photocurrent action spectra. Size-selective photoexcitation of the arrays of multiple sizes of QDs helped to determine (i) the location of the interface at which photoinduced separation of charge occurred, (ii) whether the energy absorbed by the QDs was redistributed before separation of charge, and (iii) the dependence of the photovoltage on the locations of various sizes of QDs within the junction. This research is a step toward the use of QDs for harvesting light and for transporting energy and charge in devices-for example, solar cells and photodetectors-that operate at zero bias.