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In this work, we demonstrate that an external pressure of 15–30 kPa can significantly improve metal halide perovskite (MHP) film thermal stability. We demonstrate this through the application of weight on top of an MHP film during thermal aging in preserving the perovskite phase and the mobile ion concentration, an effect which we hypothesize reduces the extent to which volatile species can escape from the MHP lattice. This method is shown to be effective for a more scalable approach by only applying the weight to a cover glass during the lamination of an epoxy-based resin, after which the weight is removed. The amount of pressure applied during lamination is shown to correlate with stability in both 1 sun illumination and damp heat testing. Lastly, the performance of MHP photovoltaic devices is improved using pressure during lamination, an effect which is attributed to improved interfacial contact between the MHP and the adjacent charge transport layers and healing of any voids or defects that may exist at the buried interface after processing. As such, there are implications for tuning the amount of pressure that is applied during lamination to enable the durability of MHP solar modules toward manufacturing-scale deployment. 

Abstract Hybrid metal halide perovskite (MHP) materials, while being promising for photovoltaic technology, also encounter challenges related to material stability. Combining 2D MHPs with 3D MHPs offers a viable solution, yet there is a gap in the understanding of the stability among various 2D materials. The mechanical, ionic, and environmental stability of various 2D MHP ligands are reported, and an improvement with the use of a quater‐thiophene‐based organic cation (4TmI) that forms an organic‐semiconductor incorporated MHP structure is demonstrated. It is shown that the best balance of mechanical robustness, environmental stability, ion activation energy, and reduced mobile ion concentration under accelerated aging is achieved with the usage of 4TmI. It is believed that by addressing mechanical and ion‐based degradation modes using this built‐in barrier concept with a material system that also shows improvements in charge extraction and device performance, MHP solar devices can be designed for both reliability and efficiency. 

We report on the use of open-air blade-coating as a scalable method for producing metal halide perovskite films with >10× fracture energy for durability and mechanical stability through the addition of corn starch polymer additives. This results in a manufacturable and robust perovskite that has tunable thicknesses exceeding 10 µm, among the highest reported values for solution-processed polycrystalline films. We find that an increasing amount of starch causes more uniform carbon distribution within the perovskite thickness as quantified by cross-sectional elemental composition measurements. Further, the incorporation of starch introduces beneficial compressive film stresses. Importantly, the optoelectronic behavior is not compromised, as the photoluminescence spectrum becomes more homogenous with the addition of corn starch up to 20% by weight. 

We report on the use of 2D Ruddlesden–Popper (RP) perovskites as optoelectronic materials in building-integrated applications, addressing the challenge of balancing transparency, photoluminescence, and stability. With the addition of polyvinylpyrrolidone (PVP), the 2D RP films exhibit superior transparency compared to their 3D counterparts with an average visible transmittance (AVT) greater than 50% and photoluminescence stability under continuous illumination and 85 °C heat for up to 100 h as bare, unencapsulated films. Structural investigations show a stress relaxation in the 3D perovskite films after degradation from thermal aging that is not observed in the 2D RP films, which retain their phase after thermal and light aging. We also demonstrate ultrasmooth, wide-bandgap 2D Dion–Jacobson (DJ) films with PVP incorporation up to 2.95 eV, an AVT above 70%, and roughnesses of ~2 nm. These findings contribute to the development of next-generation solar materials, paving the way for their integration into built structures. 

We report on the use of an atmospheric pressure, open-air plasma treatment to remove Li2CO3 species from the surface of garnet-type tantalum-doped lithium lanthanum zirconium oxide (Li6.4La3Zr1.4Ta0.6O12, LLZTO) solid-state electrolyte pellets. The Li2CO3 layer, which we show forms on the surface of garnets within 3 min of exposure to ambient moisture and CO2, increases the interface (surface) resistance of LLZTO. The plasma treatment is carried out entirely in ambient and is enabled by use of a custom-built metal shroud that is placed around the plasma nozzle to prevent moisture and CO2 from reacting with the sample. After the plasma treatment, N2 compressed gas is flowed through the shroud to cool the sample and prevent atmospheric species from reacting with the LLZTO. We demonstrate that this approach is effective for removing the Li2CO3 from the surface of LLZTO. The surface chemistry is characterized with X-ray photoelectron spectroscopy to evaluate the effect of process parameters (plasma exposure time and shroud gas chemistry) on removal of the surface species. We also show that the open-air plasma treatment can significantly reduce the interface resistance. This platform demonstrates a path towards open-air processed solid-state batteries. 

Although C₆₀is usually the electron transport layer (ETL) in inverted perovskite solar cells, its molecular nature of C₆₀leads to weak interfaces that lead to non-ideal interfacial electronic and mechanical degradation. Here, we synthesized an ionic salt from C₆₀, 4-(1',5′-dihydro-1'-methyl-2'H-[5,6] fullereno-C₆₀-I_h-[1,9-c]pyrrol-2'-yl) phenylmethanaminium chloride (CPMAC), and used it as the electron shuttle in inverted PSCs. The CH₂-NH₃⁺head group in the CPMA cation improved the ETL interface and the ionic nature enhanced the packing, leading to ~3-fold increase in the interfacial toughness compared to C₆₀. Using CPMAC, we obtained ~26% power conversion efficiencies (PCEs) with ~2% degradation after 2,100 hours of 1-sun operation at 65°C. For minimodules (four subcells, 6 centimeters square), we achieved the PCE of ~23% with <9% degradation after 2,200 hours of operation at 55°C. 

We report on an examination of mobile ion concentration (N₀) in perovskite solar cells (PSCs) as a function of temperature and device architecture.