Shape-morphing nanocomposite origami.

Nature provides a vast array of solid materials that repeatedly and reversibly transform in shape in response to environmental variations. This property is essential, for example, for new energy-saving technologies, efficient collection of solar radiation, and thermal management. Here we report a similar shape-morphing mechanism using differential swelling of hydrophilic polyelectrolyte multilayer inkjets deposited on an LBL carbon nanotube (CNT) composite. The out-of-plane deflection can be precisely controlled, as predicted by theoretical analysis. We also demonstrate a controlled and stimuli-responsive twisting motion on a spiral-shaped LBL nanocomposite. By mimicking the motions achieved in nature, this method offers new opportunities for the design and fabrication of functional stimuli-responsive shape-morphing nanoscale and microscale structures for a variety of applications.

Inkjet deposition of layer-by-layer assembled films.

Layer-by-layer assembly (LBL) can create advanced composites with exceptional properties unavailable by other means, but the laborious deposition process and multiple dipping cycles hamper their utilization in microtechnologies and electronics. Multiple rinse steps provide both structural control and thermodynamic stability to LBL multilayers, but they significantly limit their practical applications and contribute significantly to the processing time and waste. Here we demonstrate that by employing inkjet technology one can deliver the necessary quantities of LBL components required for film buildup without excess, eliminating the need for repetitive rinsing steps. This feature differentiates this approach from all other recognized LBL modalities. Using a model system of negatively charged gold nanoparticles and positively charged poly(diallyldimethylammonium) chloride, the material stability, nanoscale control over thickness, and particle coverage offered by the inkjet LBL technique are shown to be equal or better than the case of multilayers made with traditional dipping cycles. The opportunity for fast deposition of complex metallic patterns using a simple inkjet printer is also shown. The additive nature of LBL deposition based on the formation of insoluble nanoparticle-polyelectrolyte complexes of various compositions provides an excellent opportunity for versatile, multicomponent, and noncontact patterning for the simple production of stratified patterns that are much needed in advanced devices.

Traversing Material Scales: Macroscale LBL-Assembled Nanocomposites with Microscale Inverted Colloidal Crystal Architecture.

The introduction of three-dimensional (3D) architecture to functional materials allows for the addition of unique characteristics such as special deformation patterns, negative Poison's ratio, negative thermal expansion, controlled biological interactions, and mass transport properties. It also aids in bridging the dimensional gap between layer-by-layer (LBL) assembled nanocomposites and macroscale applications while retaining the advantages of their nanoscale organization. Fabrication of 3D microscale features by traditional techniques are often restricted to a limited variety of materials and do not include hybrid organic-inorganic nanocomposites. This work describes a new method to synthesize macroscale materials with hierarchically controlled architecture by using LBL deposition in the voids of hexagonally packed arrays of uniform microspheres and can be potentially extended to a large variety of materials. Establishing systematic techniques to produce materials with hierarchical architecture involving nano-, micro-, and potentially millimeter scale features with fairly independent control at all levels, allows for the investigation of structural influences on material properties and for the development of new practical applications due to the unusual combinations of properties that can be achieved.

Nanocomposite microcontainers.

Versatile all-nanocomposite capped microcontainers are made using layer-by-layer (LBL) assembly. The microcontainers can act as inert packaging with slow/controlled release for virtually any type of encapsulating material based on clay nanocomposites 3D molded by PDMS templates and capped with another LBL film.

Pseudonegative thermal expansion and the state of water in graphene oxide layered assemblies.

Unraveling the complex interplay between thermal properties and hydration is a part of understanding the fundamental properties of many soft materials and very essential for many applications. Here we show that graphene oxide (GO) demonstrates a highly negative thermal expansion (NTE) coefficient owing to unique thermohydration processes related with fast transport of water between the GO sheets, the amphiphilic nature of nanochannels, and close-to-zero intrinsic thermal expansion of GO. The humidity-dependent NTE of GO layered assemblies, or "pseudonegative thermal expansion" (PNTE), differs from that of other hygroscopic materials due to its relatively fast and highly reversible expansion/contraction cycles and occurrence at low humidity levels while bearing similarities to classic NTE. Thermal expansion of polyvinyl alcohol/GO composites is easily tunable with additional intricacy of thermohydration effects. PNTE combined with isotropy, nontoxicity, and mechanical robustness is an asset for applications of actuators, sensors, MEMS devices, and memory materials and crucial for developing methods of thermal/photopatterning of GO devices.