title: Selective transformations between nanoparticle superlattices via the reprogramming of DNA-mediated interactions.
abstract: The rapid development of self-assembly approaches has enabled the creation of materials with desired organization of nanoscale components. However, achieving dynamic control, wherein the system can be transformed on demand into multiple entirely different states, is typically absent in atomic and molecular systems and has remained elusive in designed nanoparticle systems. Here, we demonstrate with in situ small-angle X-ray scattering that, by using DNA strands as inputs, the structure of a three-dimensional lattice of DNA-coated nanoparticles can be switched from an initial 'mother' phase into one of multiple 'daughter' phases. The introduction of different types of reprogramming DNA strands modifies the DNA shells of the nanoparticles within the superlattice, thereby shifting interparticle interactions to drive the transformation into a particular daughter phase. Moreover, we mapped quantitatively with free-energy calculations the selective reprogramming of interactions onto the observed daughter phases.
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: Yugang
authors.initials: Y
authors.lastname: Zhang
authors.affiliation: 1] Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA [2] Department of Chemical Engineering, Columbia University, New York, New York 10027, USA.
authors.forename: Suchetan
authors.initials: S
authors.lastname: Pal
authors.affiliation: Department of Chemical Engineering, Indian Institute of Technology Gandhinagar, Ahmedabad 682525, India.
authors.forename: Babji
authors.initials: B
authors.lastname: Srinivasan
authors.affiliation: Department of Chemical Engineering, Columbia University, New York, New York 10027, USA.
authors.forename: Thi
authors.initials: T
authors.lastname: Vo
authors.affiliation: Department of Chemical Engineering, Columbia University, New York, New York 10027, USA.
authors.forename: Sanat
authors.initials: S
authors.lastname: Kumar
authors.affiliation: Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: Oleg
authors.initials: O
authors.lastname: Gang
mesh_terms: D003460:Crystallization; D004247:DNA / Q000737:chemistry* / Q000648:ultrastructure; D006046:Gold; D053768:Metal Nanoparticles / Q000737:chemistry / Q000648:ultrastructure; D008958:Models, Molecular; D053758:Nanoparticles / Q000737:chemistry* / Q000648:ultrastructure; D036103:Nanotechnology; D044367:Phase Transition; D053838:Scattering, Small Angle; D014961:X-Ray Diffraction
chemical_list: D006046:Gold; D004247:DNA