Viscoelastic properties of ring-linear DNA blends exhibit nonmonotonic dependence on blend composition

Abstract

Entangled ring polymers, along with blends of ring and linear polymers, continue to be a topic of great interest and debate due to the conflicting experimental results in the literature as well as the difficulty of producing entangled synthetic rings devoid of linear contaminants. Here, we create blended solutions of entangled ring and linear DNA with varying mass fractions of linear DNA φL. We use optical tweezers microrheology to measure the linear and nonlinear viscoelastic response of these blends. Our measurements reveal a strong nonmonotonic dependence of linear viscoelastic properties on φL, with a pronounced maximum when the mass fraction of rings and linear chains are comparable, suggestive of pervasive threading of rings by linear chains. We observe a similar nonmonotonicity in the nonlinear regime. However, a comparatively higher fraction of linear chains (φL≈0.5-0.7) is required for a substantial increase in resisitive force and slowing of relaxation dynamics to emerge. This nonlinear response also appears to be rate dependent, which we argue arises from force-induced dethreading of rings at high strain rates. Our results fill a long-standing gap in knowledge regarding the microrheology and nonlinear response of ring-linear polymer blends. Moreover, the uniquely strong mechanical response that ring-linear blends exhibit, along with the ability to finely tune these blends by varying the blend composition, provides intriguing materials design principles.