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 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.

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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.

The refractive indices of naturally occurring materials are limited, and there exists an index gap between indices of air and available solid materials. With many photonics and electronics applications, there has been considerable effort in creating artificial materials with optical and dielectric properties similar to air while simultaneously being mechanically stable to bear load. Here, a class of ordered nanolattice materials consisting of periodic thin‐shell structures with near‐unity refractive index and high stiffness is demonstrated. Using a combination of 3D nanolithography and atomic layer deposition, these ordered nanostructured materials have reduced optical scattering and improved mechanical stability compared to existing randomly porous materials. Using ZnO and Al2O3 as the building materials, refractive indices from 1.3 down to 1.025 are achieved. The experimental data can be accurately described by Maxwell Garnett effective media theory, which can provide a guide for index design. The demonstrated low‐index, low‐scattering, and high‐stiffness materials can serve as high‐quality optical films in multilayer photonic structures, waveguides, resonators, and ultra‐low‐k dielectrics.

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.