Magnetically responsive polymer nanopillars with nickel cap.

Embedding magnetic particles within polymer matrix is a common and facile method to fabricate magnetically responsive micro-/nanoscale pillars. However, the balance between mechanical compliance and magnetic susceptibility cannot be decoupled and the particles are limited by the pillar feature size, which can limit the actuation performance. Here we demonstrate a new type of magnetically responsive nanostructure consisting of a polydimethylsiloxane (PDMS) nanopillar array with deposited nickel caps, that has successfully achieved such decoupling with multiple cap-geometry designs for a better actuation control. The actuation result of nanopillars with 540 nm period and 1.3 µm height has been analyzed using image processing, leading to a maximum displacement of 180 nm with a ratio of 13.9% with respect to the pillar height. Magnetic and mechanical models based on magnetic force and torque have been developed and used to mitigate the weakening effect of the actuation by the residual magnetic layer. This structure demonstrates a feasible strategy for magnetic actuation at the sub-micrometer scale with freedom to design magnetic cap and polymeric pillar separately. This structure can also be utilized in multiple applications such as tunable optical elements, dynamic droplet manipulation, and responsive particle manipulation.

Recent progress in near-field nanolithography using light interactions with colloidal particles: from nanospheres to three-dimensional nanostructures.

The advance of nanotechnology is firmly rooted in the development of cost-effective, versatile, and easily accessible nanofabrication techniques. The ability to pattern complex two-dimensional and three-dimensional nanostructured materials are particularly desirable, since they can have novel physical properties that are not found in bulk materials. This review article will report recent progress in utilizing self-assembly of colloidal particles for nanolithography. In these techniques, the near-field interactions of light and colloids are the sole mechanisms employed to generate the intensity distributions for patterning. Based on both 'bottom-up' self-assembly and 'top-down' lithography approaches, these processes are highly versatile and can take advantage of a number of optical effects, allowing the complex 3D nanostructures to be patterned using single exposures. There are several key advantages including low equipment cost, facile structure design, and patterning scalability, which will be discussed in detail. We will outline the underlying optical effects, review the geometries that can be fabricated, discuss key limitations, and highlight potential applications in nanophotonics, optoelectronic devices, and nanoarchitectured materials.

Twin photonic nanojets generated from coherent illumination of microscale sphere and cylinder.

Photonic nanojets, highly focused beams of light created by planar illumination of a microsphere, have been shown to produce narrow subwavelength beams over distances of several wavelengths in the near field. In this work, we investigate the generation of twin photonic nanojets through the illumination of a microsphere or cylinder from two coherent sources with relative phase shift. Under these conditions, symmetric twin nanojets separated by an intensity null can be generated. Compared to a photonic nanojet, the twin nanojets can achieve an even smaller subwavelength beam, and have the added advantage of having more complex intensity profiles that can be controlled by multiple parameters. Using both finite-difference time-domain and Mie theory models, the width, length, and intensity enhancement factor of the nanojet geometry are found to be functions of the phase, angle offsets, and particle geometry. Such twin photonic nanojets can find applications in optical trapping, manipulation, nanolithography, and enhancement of nonlinear optical properties.

Nanostructured antireflective in-plane solar harvester.

In this work, we demonstrate a two-dimensional nano-hole array that can reduce reflection losses while passively trapping and harvesting incident light. The surface structure is designed to scavenge a small portion of incident light that would typically be lost due to Fresnel reflection, while the majority of light transmits unobstructed like a regular window. The trapping mechanism is dependent on angle and wavelength, and can be designed to selectively trap narrow wavelength bands using the constructed theoretical models. We demonstrate that structures with periods of 275 nm and 325 nm can trap different wavelength range within the visible spectrum, while simultaneously suppressing reflection losses. The trapping effect can be observed visually, and can be converted to a current output using a photovoltaic (PV) cell on the glass edge. The fabrication of such materials employs a simple replication process, and can be readily scaled up for large-scale manufacturing. The demonstrated solar harvester can be potentially be widely deployed in residential and commercial buildings as multifunctional windows for solar energy harvesting, scavenging, spectra splitting, and anti-glare properties.

Enhanced total internal reflection using low-index nanolattice materials.

Low-index materials are key components in integrated photonics and can enhance index contrast and improve performance. Such materials can be constructed from porous materials, which generally lack mechanical strength and are difficult to integrate. Here we demonstrate enhanced total internal reflection (TIR) induced by integrating robust nanolattice materials with periodic architectures between high-index media. The transmission measurement from the multilayer stack illustrates a cutoff at about a 60° incidence angle, indicating an enhanced light trapping effect through TIR. Light propagation in the nanolattice material is simulated using rigorous coupled-wave analysis and transfer matrix methods, which agrees well with experimental data. The demonstration of the TIR effect in this Letter serves as a first step towards the realization of multilayer devices with nanolattice materials as robust low-index components. These nanolattice materials can find applications in integrated photonics, antireflection coatings, photonic crystals, and low-k dielectric.

Three-dimensional colloidal lithography.

Light interactions with colloidal particles can generate a variety of complex three-dimensional (3D) intensity patterns, which can be utilized for nanolithography. The study of particle-light interactions can add more types of intensity patterns by manipulating key factors. Here we investigate a novel 3D nanolithography technique using colloidal particles under two-beam coherent illuminations. The fabricated 3D nanostructures are hollow, nested within periodic structures, and possess multiple chamber geometry. The effects of incident angles and particle size on the fabricated nanostructures were examined. The relative phase shift between particle position and interference pattern is identified as another significant parameter influencing the resultant nanostructures. A numerical model has been developed to show the evolution of nanostructure geometry with phase shifts, and experimental studies confirm the simulation results. Through the introduction of single colloidal particles, the fabrication capability of Lloyd's mirror interference can now be extended to fabrication of 3D nanostructure with complex shell geometry. The fabricated hollow nanostructures with grating background could find potential applications in the area of photonics, drug delivery, and nanofluidics.

Designing unit cell in three-dimensional periodic nanostructures using colloidal lithography.

Colloidal phase-shift lithography, the illumination of a two-dimensional (2D) ordered array of self-assembled colloidal nanospheres, is an effective method for the fabrication of periodic three-dimensional (3D) nanostructures. In this work, we investigate the design and control of the unit-cell geometry by examining the relative ratio of the illumination wavelength and colloidal nanosphere diameter. Using analytical and finite-difference time-domain (FDTD) modeling, we examine the effect of the wavelength-diameter ratio on intensity pattern, lattice constants, and unit-cell geometry. These models were validated by experimental fabrication for various combination of wavelength and colloid diameter. The developed models and fabrication tools can facilitate the design and engineering of 3D periodic nanostructure for photonic crystals, volumetric electrodes, and porous materials.

Sculpting asymmetric, hollow-core, three-dimensional nanostructures using colloidal particles.

Colloidal elements have historically played a key role in "bottom-up" self-assembly processes for nanofabrication. However, these elementary components can also interact with light to generate complex intensity distributions and facilitate "top-down" lithography. Here, a nanolithography technique is demonstrated based on oblique illuminations of colloidal particles to fabricate hollow-core 3D nanostructures with complex symmetry. The light-particle interaction generates an angular light distribution as governed by Mie scattering, which can be compounded by multiple illuminations to sculpt novel 3D structures in the underlying photoresist. The fabricated geometry can be controlled by the particle parameters and illumination configurations, enabling the fabrication of a large variety of asymmetric hollow nanostructures. The proposed technique has high pattern versatility, is low cost and high throughput, and can find potential application in nanoneedles, nanonozzles, and materials with anisotropic properties.

Antireflection effects at nanostructured material interfaces and the suppression of thin-film interference.

Thin-film interference is a well-known effect, and it is commonly observed in the colored appearance of many natural phenomena. Caused by the interference of light reflected from the interfaces of thin material layers, such interference effects can lead to wavelength and angle-selective behavior in thin-film devices. In this work, we describe the use of interfacial nanostructures to eliminate interference effects in thin films. Using the same principle inspired by moth-eye structures, this approach creates an effective medium where the index is gradually varying between the neighboring materials. We present the fabrication process for such nanostructures at a polymer-silicon interface, and experimentally demonstrate its effectiveness in suppressing thin-film interference. The principle demonstrated in this work can lead to enhanced efficiency and reduce wavelength/angle sensitivity in multilayer optoelectronic devices.

Three-Dimensional Photoengraving of Monolithic, Multifaceted Metasurfaces.

Metasurfaces present a potent platform to manipulate light by the spatial arrangement of sub-wavelength patterns with well-defined sizes and geometries, in thin films. Metasurfaces by definition are planar. However, it would be highly desirable to integrate metasurfaces with diverse, spatially programmed sub-wavelength features into a 3D monolith, to manipulate light within a compact 3D space. Here, a 3D photoengraving strategy is presented; that is, generation of such composite metasurfaces from a single microstructure via the irradiation of multiple interference laser beams onto different facets of the parent azopolymeric microstructure. Through "photofluidization," this technique enables independent inscription and erasing of metasurfaces onto and from individual facets of 3D monoliths with arbitrary shapes and dimensions, in a high-throughput fashion (over approximately a few cm2 at a time). By engraving discrete sub-wavelength 1D surface relief gratings of different pitches on different facets of an inverse pyramidal array, a multiplexing structure-color filter is demonstrated.

Active Periodic Magnetic Nanostructures with High Aspect Ratio and Ultrahigh Pillar Density.

Magnetically actuated micro/nanoscale pillars have attracted significant research interest recently because of their dynamic properties. These structures can be used for various applications, such as dry adhesion, cell manipulation, and sensors or actuators in microfluidics. Magnetically actuated structures can be fabricated by mixing magnetic particles and polymers to yield a favorable combination of magnetic permeability and mechanical compliance. However, the pillar density of demonstrated structures is relatively low, which limits the potential applications in active surface manipulation of microscale objects. Here, we demonstrate active periodic nanostructures with a pillar density of 0.25 pillar/µm2, which is the highest density for magnetically actuated pillars so far. Having a structure period of 2 µm, diameter of 600 nm, and high aspect ratio of up to 11, this structure can be magnetically actuated with a displacement of up to 200 nm. The behaviors of the pillars under various cyclic actuation modes have been characterized, demonstrating that the actuation can be well controlled. This work can find potential applications in particle manipulation and tunable photonic elements.

Scalable Manufacturing of Bending-Induced Surface Wrinkles.

The wide range of textures that can be generated via wrinkling can imbue surfaces with functionalities useful for a variety of applications including tunable optics, stretchable electronics, and coatings with controlled wettability and adhesion. Conventional methods of wrinkle fabrication rely on batch processes in piece-by-piece fashion, not amenable for scale-up to enable commercialization of surface wrinkle-related technologies. In this work, a scalable manufacturing method for surface wrinkles is demonstrated on a cylindrical support using bending-induced strains. A bending strain is introduced to a thin layer of ultraviolet-curable poly(dimethylsiloxane) (UV-PDMS) coated on top of a soft PDMS substrate by wrapping the bilayer around a cylindrical roller. After curing the UV-PDMS and subsequently releasing the bending strain, one-dimensional or checkerboard surface wrinkles are produced. Based on experimental and computational analyses, we show that these patterns form as a result of the interplay between swelling and bending strains. The feasibility of continuous manufacturing of surface wrinkles is demonstrated by using a two-roller roll-to-roll prototype, which paves the way for scalable roll-to-roll processing. To demonstrate the utility of these textures, we show that surface wrinkles produced in this manner enhance the light harvesting and thus efficiency of a solar cell at oblique angles of illumination due to their strong light scattering properties.

Quantitative infrared spectroscopy of environmentally sensitive and rough materials.

Fourier transform infrared (FTIR) spectroscopy is a widely used characterization technique for studying chemical compositions and light-matter interactions in the infrared range. However, it remains challenging to use conventional FTIR equipment to characterize materials that are environmentally sensitive and/or have rough surfaces due to their dynamic response to external stimuli (e.g., humidity) and light scattering from the sample surface. Here, we describe an approach enabling quantitative infrared spectroscopy measurements of these challenging samples, including transmittance, reflectance, and emissivity. We designed and 3D-printed a miniaturized environmental chamber that can be directly inserted into the sample holder of a conventional integrating sphere to perform total transmission and reflection measurements in controlled environments. Moreover, a calibration method was developed to exclude light scattering from rough surfaces of the sample and the distortion created by infrared windows. To illustrate the potential application of this method, we have performed quantitative infrared measurements, both specular and diffusive, on a sapphire standard reference with a specular surface, as well as a textile sample that has a rough surface and is dynamically responsive to changes in humidity. The calibrated results measured with the equipped chamber match those measured without the IR windows, demonstrating the viability of our environmental chamber and the proposed calibration method. This quantitative infrared spectroscopy measurement technique may help advance fields such as metasurfaces and adaptive textiles, where samples are often rough, dynamically responsive, and/or environmentally sensitive.

Dynamic gating of infrared radiation in a textile.

The human body absorbs and loses heat largely through infrared radiation centering around a wavelength of 10 micrometers. However, neither our skin nor the textiles that make up clothing are capable of dynamically controlling this optical channel for thermal management. By coating triacetate-cellulose bimorph fibers with a thin layer of carbon nanotubes, we effectively modulated the infrared radiation by more than 35% as the relative humidity of the underlying skin changed. Both experiments and modeling suggest that this dynamic infrared gating effect mainly arises from distance-dependent electromagnetic coupling between neighboring coated fibers in the textile yarns. This effect opens a pathway for developing wearable localized thermal management systems that are autonomous and self-powered, as well as expanding our ability to adapt to demanding environments.

Photoactuated Pens for Molecular Printing.

The photoactuation of pen arrays made of polydimethylsiloxane carbon nanotube composites is explored, and the first demonstration of photoactuated pens for molecular printing is reported. Photoactuation of these composites is characterized using atomic force microscopy and found to produce microscale motion in response to modest illumination, with an actuation efficiency as high as 200 nm mW-1 on the sub-1 s time scale. Arrays of composite pens are synthesized and it is found that local illumination is capable of moving selected pens by more than 3 µm out of the plane, bringing them into contact to perform controllable and high quality printing while completely shutting off the nonilluminated counterparts. In light of the scalability limitations of nanolithography, this work presents an important step and paves the way for arbitrary control of individual pens in massive arrays. As an example of a scalable soft actuator, this approach can also aid progress in other fields such as soft robotics and microfluidics.

Large-Area Nanolattice Film with Enhanced Modulus, Hardness, and Energy Dissipation.

We present an engineered nanolattice material with enhanced mechanical properties that can be broadly applied as a thin film over large areas. The nanolattice films consist of ordered, three-dimensional architecture with thin-shell tubular elements, resulting in favorable modulus-density scaling (n ~ 1.1), enhanced energy dissipation, and extremely large material recoverability for strains up to 20% under normal compressive loading. At 95.6% porosity, the nanolattice film has demonstrated modulus of 1.19 GPa and specific energy dissipation of 325.5 kJ/kg, surpassing previously reported values at similar densities. The largest length scale in the reported nanolattice is the 500 nm unit-cell lattice constant, allowing the film to behave more like a continuum material and be visually unobservable. Fabricated using three-dimensional colloidal nanolithography and atomic layer deposition, the process can be scaled for large-area patterning. The proposed nanolattice film can find applications as a robust multifunctional insulating film that can be applied in integrated photonic elements, optoelectronic devices, and microcircuit chips.

Three-dimensional nanolithography using light scattering from colloidal particles.

The interaction between light and colloidal elements can result in a wealth of interesting near-field optical patterns. By examining the optical and colloidal properties, the intensity distribution can be tailored and harnessed for three-dimensional nanolithography. Here, we examine the use of light scattering from colloidal particles to fabricate complex hollow nanostructures. In this approach, a single colloidal sphere is illuminated to create a scattering pattern, which is captured by a photoresist in close proximity. No external optical elements are required, and the colloidal elements alone provide the modulation of the optical intensity pattern. The fabricated nanostructures can be designed to have multiple shells, confined volumes, and single top openings, resembling "nano-volcanoes." The geometry of such structures is dependent on the scattered light distribution and can be accurately modeled by examining the light-particle interaction. The hollow nanostructures can be used to trap nanomaterial, and we demonstrate their ability to trap 50 nm silica nanoparticles. These well-defined surface hollow structures can be further functionalized for applications in controlled drug delivery and biotrapping. Colloidal elements with different geometries and material compositions can also be incorporated to examine other light-colloid interactions.