Full Geometric Control of Hidden Color Information in Diffraction Gratings under Angled White Light Illumination.

Under white light illumination, gratings produce an angular distribution of wavelengths dependent on the diffraction order and geometric parameters. However, previous studies of gratings are limited to at least one geometric parameter (height, periodicity, orientation, angle of incidence) kept constant. Here, we vary all geometric parameters in the gratings using a versatile nanofabrication technique, two-photon polymerization lithography, to encode hidden color information through two design approaches. The first approach hides color information by decoupling the effects of grating height and periodicity under normal and oblique incidence. The second approach hides multiple sets of color information by arranging gratings in sectors around semicircular pixels. Different images are revealed with negligible crosstalk under oblique incidence and varying sample rotation angles. Our analysis shows that an angular separation of ≥10° between adjacent sectors is required to suppress crosstalk. This work has potential applications in information storage and security watermarks.

Stiff Shape Memory Polymers for High-Resolution Reconfigurable Nanophotonics.

Reconfigurable metamaterials require constituent nanostructures to demonstrate switching of shapes with external stimuli. Yet, a longstanding challenge is in overcoming stiction caused by van der Waals forces in the deformed configuration, which impedes shape recovery. Here, we introduce stiff shape memory polymers. This designer material has a storage modulus of ∼5.2 GPa at room temperature and ∼90 MPa in the rubbery state at 150 °C, 1 order of magnitude higher than those in previous reports. Nanopillars with diameters of ∼400 nm and an aspect ratio as high as ∼10 were printed by two-photon lithography. Experimentally, we observe shape recovery as collapsed and touching structures overcome stiction to stand back up. We develop a theoretical model to explain the recoverability of these sub-micrometer structures. Reconfigurable structural color prints with a resolution of 21150 dots per inch and holograms are demonstrated, indicating potential applications of the stiff shape memory polymers in high-resolution reconfigurable nanophotonics.

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.

Arbitrary engineering of spatial caustics with 3D-printed metasurfaces.

Caustics occur in diverse physical systems, spanning the nano-scale in electron microscopy to astronomical-scale in gravitational lensing. As envelopes of rays, optical caustics result in sharp edges or extended networks. Caustics in structured light, characterized by complex-amplitude distributions, have innovated numerous applications including particle manipulation, high-resolution imaging techniques, and optical communication. However, these applications have encountered limitations due to a major challenge in engineering caustic fields with customizable propagation trajectories and in-plane intensity profiles. Here, we introduce the "compensation phase" via 3D-printed metasurfaces to shape caustic fields with curved trajectories in free space. The in-plane caustic patterns can be preserved or morphed from one structure to another during propagation. Large-scale fabrication of these metasurfaces is enabled by the fast-prototyping and cost-effective two-photon polymerization lithography. Our optical elements with the ultra-thin profile and sub-millimeter extension offer a compact solution to generating caustic structured light for beam shaping, high-resolution microscopy, and light-matter-interaction studies.

Coloured vortex beams with incoherent white light illumination.

The orbital angular momentum is a fundamental degree of freedom of light wavefronts, currently exploited in applications where information capacity is a key requirement, such as optical communication, super-resolution imaging and high-dimensional quantum computing. However, generating orbital angular momentum beams requires spatio-temporally coherent light sources (lasers or supercontinuum sources), because incoherent light would smear out the doughnut features of orbital angular momentum beams, forming polychromatic or obscured orbital angular momentum beams instead. Here we show generation of coloured orbital angular momentum beams using incoherent white light. Spatio-temporal coherence is achieved by miniaturizing spiral phase plates and integrating them with structural colour filters, three-dimensionally printed at the nanoscale. Our scheme can in principle generate multiple helical eigenstates and combine colour information into orbital angular momentum beams independently. These three-dimensional optical elements encoded with colour and orbital angular momentum information substantially increase the number of combinations for optical anti-counterfeiting and photonic lock-key devices in a pairwise fashion.

3D-printed multilayer structures for high-numerical aperture achromatic metalenses.

Flat optics consisting of nanostructures of high-refractive index materials produce lenses with thin form factors that tend to operate only at specific wavelengths. Recent attempts to achieve achromatic lenses uncover a trade-off between the numerical aperture (NA) and bandwidth, which limits performance. Here, we propose a new approach to design high-NA, broadband, and polarization-insensitive multilayer achromatic metalenses (MAMs). We combine topology optimization and full-wave simulations to inversely design MAMs and fabricate the structures in low-refractive index materials by two-photon polymerization lithography. MAMs measuring 20 µm in diameter operating in the visible range of 400 to 800 nm with 0.5 and 0.7 NA were achieved with efficiencies of up to 42%. We demonstrate broadband imaging performance of the fabricated MAM under white light and RGB narrowband illuminations. These results highlight the potential of the 3D-printed multilayer structures for realizing broadband and multifunctional meta-devices with inverse design.

Reconfiguring Colors of Single Relief Structures by Directional Stretching.

Color changes can be achieved by straining photonic crystals or gratings embedded in stretchable materials. However, the multiple repeat units and the need for a volumetric assembly of nanostructures limit the density of information content. Inspired by surface reliefs on oracle bones and music records as a means of information archival, here, surface-relief elastomers are endowed with multiple sets of information that are accessible by mechanical straining along in-plane axes. Distinct from Bragg diffraction effects from periodic structures, trenches that generate color due to variations in trench depth, enabling individual trench segments to support a single color, are reported. Using 3D printed cuboids, trenches of varying geometric parameters are replicated in elastomers. These parameters determine the initial color (or lack thereof), the response to capillary forces, and the appearance when strained along or across the trenches. Strain induces modulation in trench depth or the opening and closure of a trench, resulting in surface reliefs with up to six distinct states, and an initially featureless surface that reveals two distinct images when stretched along different axes. The highly reversible structural colors are promising in optical data archival, anti-counterfeiting, and strain-sensing applications.

High-resolution light field prints by nanoscale 3D printing.

A light field print (LFP) displays three-dimensional (3D) information to the naked-eye observer under ambient white light illumination. Changing perspectives of a 3D image are seen by the observer from varying angles. However, LFPs appear pixelated due to limited resolution and misalignment between their lenses and colour pixels. A promising solution to create high-resolution LFPs is through the use of advanced nanofabrication techniques. Here, we use two-photon polymerization lithography as a one-step nanoscale 3D printer to directly fabricate LFPs out of transparent resin. This approach produces simultaneously high spatial resolution (29-45 µm) and high angular resolution (~1.6°) images with smooth motion parallax across 15 × 15 views. Notably, the smallest colour pixel consists of only a single nanopillar (~300 nm diameter). Our LFP signifies a step towards hyper-realistic 3D images that can be applied in print media and security tags for high-value goods.

Structural multi-colour invisible inks with submicron 4D printing of shape memory polymers.

Four-dimensional (4D) printing of shape memory polymer (SMP) imparts time responsive properties to 3D structures. Here, we explore 4D printing of a SMP in the submicron length scale, extending its applications to nanophononics. We report a new SMP photoresist based on Vero Clear achieving print features at a resolution of ~300 nm half pitch using two-photon polymerization lithography (TPL). Prints consisting of grids with size-tunable multi-colours enabled the study of shape memory effects to achieve large visual shifts through nanoscale structure deformation. As the nanostructures are flattened, the colours and printed information become invisible. Remarkably, the shape memory effect recovers the original surface morphology of the nanostructures along with its structural colour within seconds of heating above its glass transition temperature. The high-resolution printing and excellent reversibility in both microtopography and optical properties promises a platform for temperature-sensitive labels, information hiding for anti-counterfeiting, and tunable photonic devices.

Rotation-Selective Moiré Magnification of Structural Color Pattern Arrays.

When a microlens array is aligned and overlaid on an array of patterns with similar periodicity, a highly magnified image of the patterns is observed. This effect, known as moiré magnification, is used to reveal micropatterns that are unresolvable by the naked eye. These patterns are typically limited by print resolution to single color patterns. Here, we demonstrate the potential to selectively reveal more than one set of color patterns. By rotating a microlens array relative to a print containing three overlapping arrays of structural color patterns in 10° steps, each pattern array can be distinctly revealed with minimal crosstalk. This rotation-selective effect of moiré magnification is not seen in conventional microscopy. An advantage is that the moiré images are observable by the naked eye under incoherent illumination. We leverage nanoscale three-dimensional printing by using the two-photon lithography process to produce structural color pattern arrays in a single lithographic step with precisely aligned color pixels. We believe that this work can have applications in precise rotational-alignment tools, covert security documents, and information multiplexing devices.