Orthosilicic acid is the most fundamental building block of dissolved silica, which are themselves among the most ubiquitous classes of compounds found in surface waters. A thorough understanding of the chemistry of orthosilicic acid is therefore vital to elucidate phenomena involving silica such as mineralization, nutrient bioavailability, and geothermal well scaling. Unfortunately, although great effort has been expended in experiments and simulation, the dimerization reaction, which is one of the simplest of its reactions, is still not very well understood; the same can be said about the reverse reaction, or the hydrolysis of the dimer.