  Most binary superlattices created using DNA functionalization or other
approaches rely on particle size differences to achieve compositional order and
structural diversity. Here we study two-dimensional (2D) assembly of
DNA-functionalized micron-sized particles (DFPs), and employ a strategy that
leverages the tunable disparity in interparticle interactions, and thus
enthalpic driving forces, to open new avenues for design of binary
superlattices that do not rely on the ability to tune particle size (i.e.,
entropic driving forces). Our strategy employs tailored blends of complementary
strands of ssDNA to control interparticle interactions between micron-sized
silica particles in a binary mixture to create compositionally diverse 2D
lattices. We show that the particle arrangement can be further controlled by
changing the stoichiometry of the binary mixture in certain cases. With this
approach, we demonstrate the abil- ity to program the particle assembly into
square, pentagonal, and hexagonal lattices. In addition, different particle
types can be compositionally ordered in square checkerboard and hexagonal -
alternating string, honeycomb, and Kagome arrangements.
