Hydrodynamics selects the pathway for displacive transformations in DNA-linked colloidal crystallites

• DOI: 10.1073/pnas.1318012111
• Publication Date: 2014-03-18T05:41:09Z
• Authors: Ian C. Jenkins; Marie T. Casey; James T. McGinley; John C. Crocker; Talid Sinno
• Keywords: Diffusion; Chlorides; 0103 physical sciences; Hydrodynamics; Anisotropy; Cesium; Computer Simulation; Colloids; DNA; Crystallization; Vibration; 01 natural sciences; 3. Good health

Significance The use of single-stranded DNA oligomers grafted onto submicron particles to drive interparticle interactions is a versatile technique for assembly. Although progress has been made in the attainable structural complexity, whether these assemblies are kinetically arrested or dynamically reconfigurable materials is not well understood. Here, we study the mechanism responsible for recently observed diffusionless transformations in DNA-assembled colloidal crystallites. We discover that hydrodynamic forces act to establish diffusional anisotropy that selects for specific child structures, consistent with experimental observations. The notion that hydrodynamic correlations play a significant role in such transformations provides evidence that DNA-linked particle assemblies are not simple thermodynamic constructs but, like many other materials of technological interest, require the simultaneous consideration of process and properties.