A new technique is introduced to quantify microsegregation during rapid solidification. The quantification involves calculation of the average solute solubility in the primary phase during solidification of an Al-Cu binary alloy. The calculation is based on using volume percent eutectic and weight percent of second phase (in the eutectic), which were obtained experimentally. Neutron diffraction experiments and stereology calculation on scanning electron microscope images were done on impulse atomized Al-Cu alloys of three compositions (nominal), 5 wt pct Cu, 10 wt pct Cu, and 17 wt pct Cu, atomized under N 2 and He gas. Neutron diffraction experiments yielded weight percent CuAl 2 data and stereology yielded volume percent eutectic data. These two data were first used to determine the weight percent eutectic. Using the weight percent eutectic and weight percent CuAl 2 in mass and volume balance equations, the average solute solubility in the primary phase could be calculated. The experimental results of the amount of eutectic, tomography results from previous work, and results from the calculations suggest that the atomized droplets are in metastable state during the nucleation undercooling of the primary phase, and the effect of metastability propagates through to the eutectic formation stage. The metastable effect is more pronounced in alloys with higher solute composition.