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Abstract The self-assembly of DNA-coated colloids into highly-ordered structures offers great promise for advanced optical materials. However, control of disorder, defects, melting, and crystal growth is hindered by the lack of a microscopic understanding of DNA-mediated colloidal interactions. Here we use total internal reflection microscopy to measure in situ the interaction potential between DNA-coated colloids with nanometer resolution and the macroscopic melting behavior. The range and strength of the interaction are measured and linked to key material design parameters, including DNA sequence, polymer length, grafting density, and complementary fraction. We present a first-principles model that screens and combines existing theories into one coherent framework and quantitatively reproduces our experimental data without fitting parameters over a wide range of DNA ligand designs. Our theory identifies a subtle competition between DNA binding and steric repulsion and accurately predicts adhesion and melting at a molecular level. Combining experimental and theoretical results, our work provides a quantitative and predictive approach for guiding material design with DNA-nanotechnology and can be further extended to a diversity of colloidal and biological systems. 

Polymer networks consisting of a mixture of chemical and physical cross-links are known to exhibit complex time-dependent behaviour due to the kinetics of bond association and dissociation. In this article, we highlight and compare two recent physically based constitutive models that describe the nonlinear viscoelastic behaviour of such transient networks. These two models are developed independently by two groups of researchers using different mathematical formulations. Here, we show that this difference can be attributed to different viewpoints: Lagrangian versus Eulerian. We establish the equivalence of the two models under the special situation where chains obey Gaussian statistics and steady-state bond dynamics. We provide experimental data demonstrating that both models can accurately predict the time-dependent uniaxial behaviour of a poly(vinylalcohol) dual cross-link hydrogel. We review the advantages and disadvantages of both approaches in applications and close by discussing a list of open challenges and questions regarding the mathematical modelling of soft, viscoelastic networks.