Figure 5. Convective assembly processes for the two-dimensional crystallization of colloids. (a) Vertical deposition process. (b) Horizontal deposition process. (c) Typical problems arising from convective assembly processes as reported by Dimitrov et al. Reprinted with permission from ref 198.

A versatile and simple method is presented for the rapid fabrication of close‐packed colloidal 2D crystals with large domain sizes by floating and redeposition of colloidal monolayers at the air/water interface. A detailed analysis of the particle surface transformation and packing during the individual steps of the monolayer fabrication process has been conducted. It was found that the quality of the monolayer depends on parameters like colloidal particle distribution on the initial substrate, subphase pH, and addition of surfactants. The floating monolayers could be transferred and stacked onto many substrate types, regardless of surface polarity, roughness, or curvature.

We report on the observation of two hypersonic phononic gaps of different nature in three-dimensional colloidal films of nanospheres using Brillouin light scattering. One is a Bragg gap occurring at the edge of the first Brillouin zone along a high-symmetry crystal direction. The other is a hybridization gap in crystalline and amorphous films, originating from the interaction of the band of quadrupole particle eigenmodes with the acoustic effective-medium band, and its frequency position compares well with the computed lowest eigenfrequency. Structural disorder eliminates the Bragg gap, while the hybridization gap is robust.

Colloidal particles show interaction with electromagnetic radiation at optical frequencies. At the same time clever colloid design and functionalization concepts allow for versatile particle assembly providing monolayers of macroscopic dimensions. This has led to a significant interest in assembled colloidal structures for light harvesting in photovoltaic devices. In particular thin-film solar cells suffer from weak absorption of incoming photons. Consequently light management using assembled colloidal structures becomes vital for enhancing the efficiency of a given device. This review aims at giving an overview of recent developments in colloid synthesis, functionalization and assembly with a focus on light management structures in photovoltaics. We distinguish between optical effects related to the single particle properties as well as collective optical effects, which originate from the assembled structures.Colloidal templating approaches open yet another dimension for controlling the interaction with light. We focus in this respect on structured electrodes that have received much attention due to their dual functionality as light harvesting systems and conductive electrodes and highlight the impact of interparticle spacing for templating.

In this contribution, the optical losses and gains attributed to periodic nanohole array electrodes in polymer solar cells are systematically studied. For this, thin gold nanomeshes with hexagonally ordered holes and periodicities (P) ranging from 202 nm to 2560 nm are prepared by colloidal lithography. In combination with two different active layer materials (P3HT:PC61BM and PTB7:PC71BM), the optical properties are correlated with the power conversion efficiency (PCE) of the solar cells. A cavity mode is identified at the absorption edge of the active layer material. The resonance wavelength of this cavity mode is hardly defined by the nanomesh periodicity but rather by the absorption of the photoactive layer. This constitutes a fundamental dilemma when using nanomeshes as ITO replacement. The highest plasmonic enhancement requires small periodicities. This is accompanied by an overall low transmittance and high parasitic absorption losses. Consequently, larger periodicities with a less efficient cavity mode, yet lower absorptive losses were found to yield the highest PCE. Nevertheless, ITO-free solar cells reaching ~77% PCE compared to ITO reference devices are fabricated. Concomitantly, the benefits and drawbacks of this transparent nanomesh electrode are identified, which is of high relevance for future ITO replacement strategies.

Insight into the mechanical behaviour of nanomaterials under the extreme condition of very high deformation rates and to very large strains is needed to provide improved understanding for the development of new protective materials. Applications include protection against bullets for body armour, micrometeorites for satellites, and high-speed particle impact for jet engine turbine blades. Here we use a microscopic ballistic test to report the responses of periodic glassy-rubbery layered block-copolymer nanostructures to impact from hypervelocity micron-sized silica spheres. Entire deformation fields are experimentally visualized at an exceptionally high resolution (below 10 nm) and we discover how the microstructure dissipates the impact energy via layer kinking, layer compression, extreme chain conformational flattening, domain fragmentation and segmental mixing to form a liquid phase. Orientation-dependent experiments show that the dissipation can be enhanced by 30% by proper orientation of the layers.

We apply colloidal lithography to construct stacked nanocrescent dimer structures with an exact vertical alignment and a separation distance of approximately 10 nm. Highly ordered, large arrays of these nanostructures are accessible using nonclose-packed colloidal monolayers as masks. Spatially separated nanocrescent dimers are obtained by application of spatially distributed colloids. The polarization dependent optical properties of the nanostructures are investigated in detail and compared to single crescents. The close proximity of the nanocrescents leads to a coupling process that gives rise to new optical resonances which can be described as linear superpositions of the individual crescents' plasmonic modes. We apply a plasmon hybridization model to explain the spectral differences of all polarization dependent resonances and use geometric arguments to explain the respective shifts of the resonances. Theoretical calculations are performed to support the hybridization model and extend it to higher order resonances not resolved experimentally.

Hollow silica nanoparticles (HSNP) with diameters comparable to visible wavelengths and with thin shells (<15 nm) feature an unexpected color effect. Single particle and powder spectroscopy, as well as calculations based on Mie theory were used to investigate this phenomenon. The use of HSNPs increases the transport mean free path of light significantly, which reduces multiple scattering, and thus the Mie resonances become visible to the bare eye.