Reply to Soper et al.: Fluctuations in water around a bimodal distribution of local hydrogen-bonded structural motifs

Abstract

Soper et al. (1) propose that the rise in the structure factor S(Q) at low Q in the small-angle x-ray scattering (SAXS) data reported in ref. 2 is caused by stochastic number fluctuations present in all liquids and that these fluctuations are not qualitatively different for water. Water, however, exhibits enhanced number density fluctuations both at higher and lower temperatures. Clearly, the driving force cannot be the same in both temperature regimes. In ref. 2, we suggest that the balance between minimizing enthalpy (tetrahedral regions) and entropy (disordered regions) provides the driving force dominating at low temperatures and that cooperatively enhanced H bonds associated with lower-density, tetrahedral regions may play an important role.