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Functionalization of nanoparticles or colloids is increasingly being used todevelop customizable "atoms". Functionalization by attaching single strands ofDNA allows for direct control of the binding between nanoparticles, sincehybridization of double strands will only occur if the base sequences of singlestrands are complementary. Nanoparticles and colloids functionalized by foursingle strands of DNA can be thought of as designed analogs to tetrahedralnetwork forming atoms and molecules, with a difference that the attached DNAstrands allow for control of the length scale of bonding relative to the coresize. We explore the behavior of an experimentally realized model for ananoparticles functionalized by four single strands of DNA (a tetramer), andshow that this single-component model exhibits a rich phase diagram with atleast three critical points and four thermodynamically distinct amorphousphases. We demonstrate that the additional critical points are part of theIsing universality class, like the ordinary liquid-gas critical point. Thedense phases consist of a hierarchy of interpenetrating networks, reminiscentof a woven cloth. Thus bonding specificity of DNA provides an effective routeto generate new nano-networked materials with polyamorphic behavior. Theconcept of network interpenetration helps to explain the generation of multipleliquid phases in single-component systems, suggested to occur in some atomicand molecular network forming fluids, including water and silica.

Hierarchies of networked phases induced by multiple liquid-liquid critical points