Templated Assembly of Nanoparticles into Continuous Arrays

The templated assembly of nanoparticles has been limited so far to yield only discontinuous nanoparticle clusters confined within lithographically patterned cavities. Here, we explored the templated assembly of nanoparticles into continuous 2D structures, using lithographically patterned templates with topographical features sized as the assembled nanoparticles. We found that these features act as nucleation centers, whose exact arrangement determines four possible assembly regimes (i) rotated, (ii) disordered, (iii) closely packed, and (iv) unpacked. These regimes produce structures strikingly different from their geometry, orientation, long-range and short-range orders, and packing density. Interestingly, for templates with relatively distant nucleation centers, these four regimes are replaced with three new ones, which produce large monocrystalline domains that are either (i) uniformly rotated, (ii) uniformly aligned, or (iii) nonuniformly rotated relative to the nucleation lattice. We rationalized our experimental data using a mathematical model, which examines all the alignment possibilities between the nucleation centers and the ideal hexagonal assembly. Our finding provides a new approach for the à la carte obtainment of various nanoscale structures unachievable by natural self-assembly and opens a route for the fabrication of numerous functional nanodevices and nanosystems that could not be realized so far by the standard bottom-up approach.