Single-crystal Winterbottom constructions of nanoparticle superlattices

Achieving control of light-material interactions for photonic device applications at nanoscale dimensions will require structures that guide electromagnetic energy with a lateral mode confinement below the diffraction limit of light. This cannot be achieved by using conventional waveguides or photonic crystals. It has been suggested that electromagnetic energy can be guided below the diffraction limit along chains of closely spaced metal nanoparticles that convert the optical mode into non-radiating surface plasmons. A variety of methods such as electron beam lithography and self-assembly have been used to construct metal nanoparticle plasmon waveguides. However, all investigations of the optical properties of these waveguides have so far been confined to collective excitations, and direct experimental evidence for energy transport along plasmon waveguides has proved elusive. Here we present observations of electromagnetic energy transport from a localized subwavelength source to a localized detector over distances of about 0.5 microm in plasmon waveguides consisting of closely spaced silver rods. The waveguides are excited by the tip of a near-field scanning optical microscope, and energy transport is probed by using fluorescent nanospheres.

A current limitation in nanoparticle superlattice engineering is that the identities of the particles being assembled often determine the structures that can be synthesized. Therefore, specific crystallographic symmetries or lattice parameters can only be achieved using specific nanoparticles as building blocks (and vice versa). We present six design rules that can be used to deliberately prepare nine distinct colloidal crystal structures, with control over lattice parameters on the 25- to 150-nanometer length scale. These design rules outline a strategy to independently adjust each of the relevant crystallographic parameters, including particle size (5 to 60 nanometers), periodicity, and interparticle distance. As such, this work represents an advance in synthesizing tailorable macroscale architectures comprising nanoscale materials in a predictable fashion.

Colloids display intriguing transitions between gas, liquid, solid and liquid crystalline phases. Such phase transitions are ubiquitous in nature and have been studied for decades. However, the predictions of phase diagrams are not always realized; systems often become undercooled, supersaturated, or trapped in gel-like states. In many cases the end products strongly depend on the starting position in the phase diagram and discrepancies between predictions and actual observations are due to the intricacies of the dynamics of phase transitions. Colloid science aims to understand the underlying mechanisms of these transitions. Important advances have been made, for example, with new imaging techniques that allow direct observation of individual colloidal particles undergoing phase transitions, revealing some of the secrets of the complex pathways involved.