Full Color and Grayscale Painting with 3D Printed Low-Index Nanopillars.

Sculpting nanostructures into different geometries in either one or two dimensions produces a wide range of colorful elements in microscopic prints. However, achieving different shades of gray and control of color saturation remain challenging. Here, we report a complete approach to color and grayscale generation based on the tuning of a single nanostructure geometry. Through two-photon polymerization lithography, we systematically investigated color generation from the basic single nanopillar geometry in low-refractive-index (n < 1.6) material. Grayscale and full color palettes were achieved that allow decomposition onto hue, saturation, and brightness values. This approach enabled the "painting" of arbitrary colorful and grayscale images by mapping desired prints to precisely controllable parameters during 3D printing. We further extend our understanding of the scattering properties of the low-refractive-index nanopillar to demonstrate grayscale inversion and color desaturation and steganography at the level of single nanopillars.

Template-induced structure transition in sub-10 nm self-assembling nanoparticles.

We report on the directed self-assembly of sub-10 nm gold nanoparticles confined within a template comprising channels of gradually varying widths. When the colloidal lattice parameter is mismatched with the channel width, the nanoparticles rearrange and break their natural close-packed ordering, transiting through a range of structural configurations according to the constraints imposed by the channel. While much work has been done in assembling ordered configurations, studies of the transition regime between ordered states have been limited to microparticles under applied compression. Here, with coordinated experiments and Monte Carlo simulations we show that particles transit through a more diverse set of self-assembled configurations than observed for compressed systems. The new insight from this work could lead to the control and design of complex self-assembled patterns other than periodic arrays of ordered particles.

Directed self-assembly of densely packed gold nanoparticles.

Directing the self-assembly of sub-10-nm nanoparticles has been challenging because of the simultaneous requirements to achieve a densely packed monolayer and rearrange nanoparticles to assemble within a template. We met both requirements by separating the processes into two steps by first forming a monolayer of gold nanoparticles on a suitable liquid subphase of anisole and then transferring it edgewise onto a silicon substrate with a prepatterned template comprising nanoposts and nanogratings. Doing so resulted in nanoparticles that assembled in commensuration with the template design while exhibiting appreciable template-induced strain. These dense arrays of nanostructures could either be directly applied or used as lithographic masks in applications for light collection, chemical sensing, and data storage.

Holographic colour prints for enhanced optical security by combined phase and amplitude control.

Conventional optical security devices provide authentication by manipulating a specific property of light to produce a distinctive optical signature. For instance, microscopic colour prints modulate the amplitude, whereas holograms typically modulate the phase of light. However, their relatively simple structure and behaviour is easily imitated. We designed a pixel that overlays a structural colour element onto a phase plate to control both the phase and amplitude of light, and arrayed these pixels into monolithic prints that exhibit complex behaviour. Our fabricated prints appear as colour images under white light, while projecting up to three different holograms under red, green, or blue laser illumination. These holographic colour prints are readily verified but challenging to emulate, and can provide enhanced security in anti-counterfeiting applications. As the prints encode information only in the surface relief of a single polymeric material, nanoscale 3D printing of customised masters may enable their mass-manufacture by nanoimprint lithography.