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Abstract The in‐plane packing of gold (Au), polystyrene (PS), and silica (SiO₂) spherical nanoparticle (NP) mixtures at a water–oil interface is investigated in situ by UV–vis reflection spectroscopy. All NPs are functionalized with carboxylic acid such that they strongly interact with amine‐functionalized ligands dissolved in an immiscible oil phase at the fluid interface. This interaction markedly increases the binding energy of these nanoparticle surfactants (NPSs). The separation distance between the Au NPSs and Au surface coverage are measured by the maximum plasmonic wavelength (λ_max) and integrated intensities as the assemblies saturate for different concentrations of non‐plasmonic (PS/SiO₂) NPs. As the PS/SiO₂content increases, the time to reach intimate Au NP contact also increases, resulting from their hindered mobility. λ_maxchanges within the first few minutes of adsorption due to weak attractive inter‐NP forces. Additionally, a sharper peak in the reflection spectrum at NP saturation reveals tighter Au NP packing for assemblies with intermediate non‐plasmonic NP content. Grazing incidence small angle X‐ray scattering (GISAXS) and scanning electron microscopy (SEM) measurements confirm a decrease in Au NP domain size for mixtures with larger non‐plasmonic NP content. The results demonstrate a simple means to probe interfacial phase separation behavior using in situ spectroscopy as interfacial structures densify into jammed, phase‐separated NP films. 

We present a design strategy for fabricating ultrastable phase-pure films of formamidinium lead iodide (FAPbI₃) by lattice templating using specific two-dimensional (2D) perovskites with FA as the cage cation. When a pure FAPbI₃precursor solution is brought in contact with the 2D perovskite, the black phase forms preferentially at 100°C, much lower than the standard FAPbI₃annealing temperature of 150°C. X-ray diffraction and optical spectroscopy suggest that the resulting FAPbI₃film compresses slightly to acquire the (011) interplanar distances of the 2D perovskite seed. The 2D-templated bulk FAPbI₃films exhibited an efficiency of 24.1% in a p-i-n architecture with 0.5–square centimeter active area and an exceptional durability, retaining 97% of their initial efficiency after 1000 hours under 85°C and maximum power point tracking.