DNA Cholesteric Pitch as a Function of Density and Ionic Strength

The nature of chiral interactions among chiral biopolymers, such as DNA, protein α-helices, and rodlike virus particles, remains elusive. In particular, a satisfactory model connecting molecular chiral interactions and the pitch of the resulting chiral mesophases is lacking. We report the measurement of short-fragment (146-bp) DNA cholesteric spherulite pitch as a function of osmotic pressure, average DNA interaxial spacing, and salt concentration. We determined cholesteric pitch and interaxial spacing by polarizing optical microscopy and x-ray scattering, respectively, from which the twist-angle between DNA molecules can be calculated. Surprisingly, we found that decreasing ionic strength resulted in weaker chiral interactions between DNA chains, as evidenced by the decrease in the twist-angle, and consequent increase in the cholesteric pitch, for a fixed interaxial spacing. We propose that this behavior can be explained by increased smearing-out of the helical charge pattern along DNA as the Debye screening length is increased.