Hyaluronan orders water molecules in its nanoscale extended hydration shells.
basic_science · Level V
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- Record sourced from PubMed, PMID 33658208.
- Also identified by DOI 10.1126/sciadv.abf2558 and PMC identifier 7929505.
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Abstract
Hyaluronan (HA) is an anionic, highly hydrated bio-polyelectrolyte found in the extracellular environment, like the synovial fluid between joints. We explore the extended hydration shell structure of HA in water using femtosecond elastic second-harmonic scattering (fs-ESHS). HA enhances orientational water-water correlations. Angle-resolved fs-ESHS measurements and nonlinear optical modeling show that HA behaves like a flexible chain surrounded by extended shells of orientationally correlated water. We describe several ways to determine the concentration-dependent size and shape of a polyelectrolyte in water, using the amount of water oriented by the polyelectrolyte charges as a contrast agent. The spatial extent of the hydration shell is determined via temperature-dependent measurements and can reach up to 475 nm, corresponding to a length of 1600 water molecules. A strong isotope effect, stemming from nuclear quantum effects, is observed when light water (H<sub>2</sub>O) is replaced by heavy water (D<sub>2</sub>O), amounting to a factor of 4.3 in the scattered SH intensity.