Matter structured on a length scale comparable to or smaller than the wavelength of light can exhibit unusual optical properties. Particularly promising components for such materials are metal nanostructures, where structural alterations provide a straightforward means of tailoring their surface plasmon resonances and hence their interaction with light. But the top-down fabrication of plasmonic materials with controlled optical responses in the visible spectral range remains challenging, because lithographic methods are limited in resolution and in their ability to generate genuinely three-dimensional architectures. Molecular self-assembly provides an alternative bottom-up fabrication route not restricted by these limitations, and DNA- and peptide-directed assembly have proved to be viable methods for the controlled arrangement of metal nanoparticles in complex and also chiral geometries. Here we show that DNA origami enables the high-yield production of plasmonic structures that contain nanoparticles arranged in nanometre-scale helices. We find, in agreement with theoretical predictions, that the structures in solution exhibit defined circular dichroism and optical rotatory dispersion effects at visible wavelengths that originate from the collective plasmon-plasmon interactions of the nanoparticles positioned with an accuracy better than two nanometres. Circular dichroism effects in the visible part of the spectrum have been achieved by exploiting the chiral morphology of organic molecules and the plasmonic properties of nanoparticles, or even without precise control over the spatial configuration of the nanoparticles. In contrast, the optical response of our nanoparticle assemblies is rationally designed and tunable in handedness, colour and intensity-in accordance with our theoretical model.

https://www.softmatter.physik.uni-muenchen.de/publications/liedl/nature-483-2012.pdf

DNA-based self-assembly of chiral plasmonic nanostructures with tailored optical response

Two-photon excitation provides a means of activating chemical or physical processes with high spatial resolution in three dimensions and has made possible the development of three-dimensional fluorescence imaging, optical data storage, and lithographic microfabrication. These applications take advantage of the fact that the two-photon absorption probability depends quadratically on intensity, so under tight-focusing conditions, the absorption is confined at the focus to a volume of order λ3 (where λ is the laser wavelength). Any subsequent process, such as fluorescence or a photoinduced chemical reaction, is also localized in this small volume. Although three-dimensional data storage and microfabrication have been illustrated using two-photon-initiated polymerization of resins incorporating conventional ultraviolet-absorbing initiators, such photopolymer systems exhibit low photosensitivity as the initiators have small two-photon absorption cross-sections (δ). Consequently, this approach requires high laser power, and its widespread use remains impractical. Here we report on a class of π;-conjugated compounds that exhibit large δ (as high as 1, 250 × 10−50 cm4 s per photon) and enhanced two-photon sensitivity relative to ultraviolet initiators. Two-photon excitable resins based on these new initiators have been developed and used to demonstrate a scheme for three-dimensional data storage which permits fluorescent and refractive read-out, and the fabrication of three-dimensional micro-optical and micromechanical structures, including photonic-bandgap-type structures.

Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication

A key goal of metalens research is to achieve wavefront shaping of light using optical elements with thicknesses on the order of the wavelength. Such miniaturization is expected to lead to compact, nanoscale optical devices with applications in cameras, lighting, displays and wearable optics. However, retaining functionality while reducing device size has proven particularly challenging. For example, so far there has been no demonstration of broadband achromatic metalenses covering the entire visible spectrum. Here, we show that by judicious design of nanofins on a surface, it is possible to simultaneously control the phase, group delay and group delay dispersion of light, thereby achieving a transmissive achromatic metalens with large bandwidth. We demonstrate diffraction-limited achromatic focusing and achromatic imaging from 470 to 670 nm. Our metalens comprises only a single layer of nanostructures whose thickness is on the order of the wavelength, and does not involve spatial multiplexing or cascading. While this initial design (numerical aperture of 0.2) has an efficiency of about 20% at 500 nm, we discuss ways in which our approach may be further optimized to meet the demand of future applications. Controlling the geometry of each dielectric element of a nanostructured surface enables frequency-dependent group delay and group delay dispersion engineering, and the fabrication of an achromatic metalens for imaging in the visible in transmission.

/pdf/a-broadband-achromatic-metalens-for-focusing-and-imaging-in-1jmcuho99u.pdf

A broadband achromatic metalens for focusing and imaging in the visible.

Light- and ink-based three-dimensional (3D) printing methods allow the rapid design and fabrication of materials without the need for expensive tooling, dies or lithographic masks. They have led to an era of manufacturing in which computers can control the fabrication of soft matter that has tunable mechanical, electrical and other functional properties. The expanding range of printable materials, coupled with the ability to programmably control their composition and architecture across various length scales, is driving innovation in myriad applications. This is illustrated by examples of biologically inspired composites, shape-morphing systems, soft sensors and robotics that only additive manufacturing can produce.

Printing soft matter in three dimensions

Recent advancements in computational inverse-design approaches — algorithmic techniques for discovering optical structures based on desired functional characteristics — have begun to reshape the landscape of structures available to nanophotonics. Here, we outline a cross-section of key developments in this emerging field of photonic optimization: moving from a recap of foundational results to motivation of applications in nonlinear, topological, near-field and on-chip optics. Starting with a desired optical output it is possible to use computational algorithms to inverse design devices. The approach is reviewed here with an emphasis on nanophotonics.

Inverse design in nanophotonics

Femtosecond two-photon direct laser writing is used to create 100-µm-scale high-performance multi-lens objectives.

Two-photon direct laser writing of ultracompact multi-lens objectives

Liquid-filled photonic crystal fibers and optofluidic devices require infiltration with a variety of liquids whose linear optical properties are still not well known over a broad spectral range, particularly in the near infrared. Hence, dispersion and absorption properties in the visible and near-infrared wavelength region have been determined for distilled water, heavy water, chloroform, carbon tetrachloride, toluene, ethanol, carbon disulfide, and nitrobenzene at a temperature of 20 °C. For the refractive index measurement a standard Abbe refractometer in combination with a white light laser and a technique to calculate correction terms to compensate for the dispersion of the glass prism has been used. New refractive index data and derived dispersion formulas between a wavelength of 500 nm and 1600 nm are presented in good agreement with sparsely existing reference data in this wavelength range. The absorption coefficient has been deduced from the difference of the losses of several identically prepared liquid filled glass cells or tubes of different lengths. We present absorption data in the wavelength region between 500 nm and 1750 nm.

/pdf/linear-refractive-index-and-absorption-measurements-of-4rdg57gts7.pdf

Linear refractive index and absorption measurements of nonlinear optical liquids in the visible and near-infrared spectral region

Micro-optics are widely used in numerous applications, such as beam shaping, collimation, focusing and imaging. We use femtosecond 3D printing to manufacture free-form micro-optical elements. Our method gives sub-micrometre accuracy so that direct manufacturing even on single-mode fibres is possible. We demonstrate the potential of our method by writing different collimation optics, toric lenses, free-form surfaces with polynomials of up to 10th order for intensity beam shaping, as well as chiral photonic crystals for circular polarization filtering, all aligned onto the core of the single-mode fibres. We determine the accuracy of our optics by analysing the output patterns as well as interferometrically characterizing the surfaces. We find excellent agreement with numerical calculations. 3D printing of microoptics can achieve sufficient performance that will allow for rapid prototyping and production of beam-shaping and imaging devices.

/pdf/sub-micrometre-accurate-free-form-optics-by-three-21xeje5aph.pdf

Sub-micrometre accurate free-form optics by three-dimensional printing on single-mode fibres

We present a highly miniaturized camera, mimicking the natural vision of predators, by 3D-printing different multilens objectives directly onto a complementary metal-oxide semiconductor (CMOS) image sensor. Our system combines four printed doublet lenses with different focal lengths (equivalent to f = 31 to 123 mm for a 35-mm film) in a 2 × 2 arrangement to achieve a full field of view of 70° with an increasing angular resolution of up to 2 cycles/deg field of view in the center of the image. The footprint of the optics on the chip is below 300 μm × 300 μm, whereas their height is <200 μm. Because the four lenses are printed in one single step without the necessity for any further assembling or alignment, this approach allows for fast design iterations and can lead to a plethora of different miniaturized multiaperture imaging systems with applications in fields such as endoscopy, optical metrology, optical sensing, surveillance drones, or security.

https://advances.sciencemag.org/content/advances/3/2/e1602655.full.pdf

Timo Gissibl

Papers

Two-photon direct laser writing of ultracompact multi-lens objectives

Linear refractive index and absorption measurements of nonlinear optical liquids in the visible and near-infrared spectral region

Sub-micrometre accurate free-form optics by three-dimensional printing on single-mode fibres

3D-printed eagle eye: Compound microlens system for foveated imaging.

Three‐Dimensional Bichiral Plasmonic Crystals Fabricated by Direct Laser Writing and Electroless Silver Plating