The spring diatom bloom in the Arctic Ocean accounts for significant annual primary production leading to the most rapid annual drawdown of water-column pCO2. Late-winter waters in the Atlantic Arctic & Subarctic Provinces (AASP) have lower silicic acid concentrations than nitrate, which suggests diatom blooms may deplete Si before N. Here we test a facet of the hypothesis that silicic acid limitation terminates the spring diatom bloom in the AASP and the sinking of the senescent and dead diatoms helps drive carbon sequestration. During a 6-week study, diatoms bloomed and progressively consumed silicic acid to where it limited their growth. The onset of growth limitation was concurrent with the minimum pCO2 in the surface waters and increases in both the proportion of dead diatoms and the diatom assemblage sedimentation rate. Data reanalysis within the AASP shows a highly significant and positive correlation between silicic acid and pCO2 in the surface waters, but no significant relationship with nitrate and pCO2 was observed unless data were smoothed. Therefore, understanding the future of the AASP spring diatom bloom requires models that explicitly consider changes in silicic acid supply as a driver of this process.