RESUMEN
Here, we have synthesised a range of samples, with the formula (CH3NH3)1-2x(H3NC2H4NH3)xPbI3, with different levels of ethylenediammonium substitution to probe non-stoichiometry at the A-site of the perovskite. A single phase region was identified and is accompanied by a change in photophysical properties. The influence of aliovalent substitution with ethylenediammonium results in a decrease in HOMO level from -5.31 eV for x = 0 to -5.88 eV for x = 0.15.
RESUMEN
Back-contact perovskite solar cells are of great interest because they could achieve higher performance than conventional designs while also eliminating the need for transparent conductors. Current research in this field has focused on making electrode structures with reduced widths to collect charges more efficiently, but current lift-off-based fabrication techniques have struggled to achieve electrode widths smaller than 1000 nm and are difficult to implement on large areas. We demonstrate nanoimprint lithography in an etch-down procedure as a simple and easily scalable method to produce honeycomb-shaped, quasi-interdigitated electrode structures with widths as small as 230 nm. We then use electrodeposition to selectively deposit conformal coatings of a range of different hole-selective layers and explore how the efficiency of back-contact perovskite solar cells changes as the feature sizes are pushed into the nanoscale. We find that the efficiency of the resulting devices remains almost unchanged as the electrode width is varied from 230 to 2000 nm, which differs from reported device simulations. Our results suggest that reducing recombination and improving the quality of the charge transport layers, rather than reducing the minimum feature size, are likely to be the best pathway to maximizing the performance of back-contact perovskite solar cells.
RESUMEN
Photoluminescent quantum dots (QDs) are a prominent example of nanomaterials used in practical applications, especially in light-emitting and light-converting devices. Most of the current applications of QDs require formation of thin films or their incorporation in solid matrices. The choice of an appropriate host material capable of preventing QDs from degradation and developing a process of uniform incorporation of QDs in the matrix have become essential scientific and technological challenges. In this work, we developed a method of uniform incorporation of Cu-Zn-In-S (CZIS) QDs into a highly protective cross-linked polyisobutylene (PIB) matrix with high chemical resistance and low gas permeability. Our approach involves the synthesis of a methacrylate-terminated three-arm star-shaped PIB oligomeric precursor capable of quick formation of a robust 3D polymer network upon exposure to UV-light, as well as the design of a special ligand introducing short PIB chains onto the surface of the QDs, thus providing compatibility with the matrix. The obtained cross-linked QDs-in-polymer composites underwent a complex photostability test in air and under vacuum as well as a chemical stability test. These tests found that CZIS QDs in a cross-linked PIB matrix demonstrated excellent photo- and chemical stability when compared to identical QDs in widely used polyacrylate-based matrices. These results make the composites developed excellent materials for the fabrication of robust, stable and durable transparent light conversion layers.
RESUMEN
Lead-halide perovskites have attracted great attention due to their excellent optoelectronic properties, with rapid progress being made in their performance as light-emitting diodes (LEDs), photodiodes, and solar cells. Demonstrating large scale, high-resolution patterning of perovskites is a key enabling step to unlock their full potential for a range of optoelectronic applications. However, the development of a successful top-down lithography fabrication procedure has so far been hampered by the incompatibility of perovskite films with the solvents used during lithographic processes. Here, we perform a study on the effect of different lithographic solvents on perovskite films and use this insight to develop photolithography and electron-beam lithography procedures for patterning perovskite films. This procedure uses standard resists at low temperatures and achieves micron-scale features with flat tops. Furthermore, we expand this platform to produce arrays of multicolor pixels for potential commercial perovskite LED display applications.
RESUMEN
Understanding the initial ultrafast excited state dynamics of methylammonium lead iodide (MAPI) perovskite is of vital importance to enable its fullest utilisation in optoelectronic devices and the design of improved materials. Here we have combined advanced measurements of the ultrafast photoluminescence from MAPI films up to 0.6 eV above the relaxed excited state with cutting-edge advanced non-adiabatic quantum dynamics simulations, to provide a powerful unique insight into the earliest time behaviour in MAPI. Our joint experimental-theoretical approach highlights that the cooling of holes from deep in the valence band to the valence band edge is fast, occurring on a 100-500 fs timescale. Cooling of electrons from high in the conduction band to the conduction band edge, however, is much slower, on the order of 1-10 ps. Density of states calculations indicate that excited states with holes deep in the valence band are greatly favoured upon photoexcitation, and this matches well with the fast (100-500 fs) formation time for the relaxed excited state observed in our ultrafast PL measurements. Consequently we are able to provide a complete observation of the initial excited state evolution in this important prototypical material.