Reversible photo-induced performance deterioration is observed in mesoporous TiO 2 -containing devices in an inert environment. This phenomenon is correlated with the activation of deep trap sites due to astoichiometry of the metal oxide. Interestingly, in air, these defects can be passivated by oxygen adsorption. These results show that the doping of TiO 2 with aluminium has a striking impact upon the density of sub-gap states and enhances the conductivity by orders of magnitude. Dye-sensitized and perovskite solar cells employing Al-doped TiO 2 have increased device effi ciencies and signifi cantly enhanced operational device stability in inert atmospheres. This performance and stability enhancement is attributed to the substitutional incorporation of Al in the anatase lattice, "permanently" passivating electronic trap sites in the bulk and at the surface of the TiO 2 .

Periodic arrays of plasmonic nanostructures can support surface lattice resonances emerging from coupling between localized and diffractive modes. This allows the confinement of light at the nanometer scale with significantly increased resonance lifetimes as compared to those of purely localized modes. Here, we demonstrate that self‐assembly of plasmonic hybrid nanoparticles allows the simple and fast fabrication of periodic plasmonic monolayers featuring macroscopic dimensions and easily controllable lattice spacings. Electromagnetic coupling between diffractive and localized modes is significantly enhanced when the arrays are embedded in a homogeneous refractive index environment. This is realized through spin‐coating of a polymer film on top of the colloidal monolayer. Narrow surface lattice resonances are detected by far‐field extinction spectroscopy while optical microscopy reveals a homogeneous coupling strength on cm‐sized substrates. The surface lattice resonance position is changed by manipulation of the refractive index of the polymer film through the immersion into different organic solvents. Capitalizing on the thermoresponsive behavior of the polymer film we modulate the surface lattice resonance by temperature in a fully reversible, dynamic manner. The findings demonstrate the potential of colloidal self‐assembly as a bottom‐up approach for the fabrication of future nanophotonic devices.

We systematically investigated the structure formation pathways and transient morphologies involved in the formation of mesoporous membranes by the self-assembly of block copolymers during nonsolvent-induced phase separation. Using AFM, SEM, and in situ synchrotron SAXS, we mapped the topological paths and characteristic transient structures into a ternary phase diagram. We focused on the stability region of an ordered pore phase which is relevant for the generation of integral asymmetric isoporous membranes. We could identify several characteristic morphologies, i.e., spinodal networks, sphere percolation networks, ordered pore structures, and disordered and ordered cylinder arrangements together with transient structures connecting their stability regions. With given evaporation rates for the pure solvents, we calculated the corresponding composition trajectories in the phase diagram to identify suitable experimental conditions in terms of initial polymer volume fraction, solvent composition, and immersion time to trap the desired pore structure.

Silica hollow nanosphere colloidal crystals feature a uniquely well-defined structure across multiple length scales. This contribution elucidates the intricate interplay between structure and atmosphere on the effective thermal diffusivity as well as the effective thermal conductivity. Using silica hollow sphere assemblies, one can independently alter the particle geometry, the density, the packing symmetry, and the interparticle bonding strength to fabricate materials with an ultralow thermal conductivity. Whereas the thermal diffusivity decreases with increasing shell thickness, the thermal conductivity behaves inversely. However, the geometry of the colloidal particles is not the only decisive parameter for thermal insulation. By a combination of reduced packing symmetry and interparticle bonding strength, the thermal conductivity is lowered by additionally 70% down to only 8 mW m −1 K −1 in vacuum. The contribution of gaseous transport, even in these tiny pores (<200 nm), leads to minimum thermal conductivities of ≈35 and ≈45 mW m −1 K −1 for air and helium atmosphere, respectively. The influence of the individual contributions of the solid and (open-and closed-pore) gaseous conductions is further clarified by using finite element modeling. Consequently, these particulate materials can be considered as a non-flammable and dispersionprocessable alternative to commercial polymer foams.

Colloidal crystals consisting of monodisperse hollow silica spheres represent a well-defined porous material class, which features a range of interesting optical, mechanical, and thermal properties. These hierarchically structured materials comprise micropores within the silica network, which are confined to a thin shell (tens of nanometers) of a hollow sphere (hundreds of nanometers). Using simple calcination steps, we markedly change the internal microstructure, which we investigate by a multitude of characterization techniques, while the meso- and macrostructure remains constant. Most importantly the rearrangement of the silica condensation network leads to a reduction in the total surface area and loss of micropores as demonstrated by N2 sorption and hyperpolarized (129)Xe NMR studies. Spin-lattice relaxation shows a drastic increase of the rigidity of the amorphous network. These microstructural changes significantly influence the thermal conductivity through such a porous silica material. We demonstrate a remarkably low thermal conductivity of only 71 mW m(-1) K(-1) for a material of a comparatively high density of 1.04 kg m(-3) at 500 °C calcination temperature. This thermal conductivity increases up to 141 mW m(-1) K(-1) at the highest calcination temperature of 950 °C. The great strength of hollow silica sphere colloidal crystals lies in their hierarchical structure control, which allows further investigation of how the internal microstructure and the interfacial contact points affect the transport of heat.