The effects of changing the charge-bearing atom in the polar head of a surfactant ion on micelle size and dye solubilization efficiency were investigated. Replacement of nitrogen in decyltrimethylammonium bromide by phosphorus or arsenic increases the micellar aggregation number by at least 20% in 0.5 m NaBr solutions. The ability of the surfactants to solubilize the dye Orange-OT is only slightly affected by the substitution of phosphorus for nitrogen, but it is lowered appreciably by the substitution of arsenic.