Nicholas Rolston

Inverted (pin) perovskite solar cells (PSCs) afford improved operating stability in comparison to their nip counterparts but have lagged in power conversion efficiency (PCE). The energetic losses responsible for this PCE deficit in pin PSCs occur primarily at the interfaces between the perovskite and the charge-transport layers. Additive and surface treatments that use passivating ligands usually bind to a single active binding site: This dense packing of electrically resistive passivants perpendicular to the surface may limit the fill factor in pin PSCs. We identified ligands that bind two neighboring lead(II) ion (Pb 2+ ) defect sites in a planar ligand orientation on the perovskite. We fabricated pin PSCs and report a certified quasi–steady state PCE of 26.15 and 24.74% for 0.05– and 1.04–square centimeter illuminated areas, respectively. The devices retain 95% of their initial PCE after 1200 hours of continuous 1 sun maximum power point operation at 65°C.

Abstract An overlooked factor affecting stability: the residual stresses in perovskite films, which are tensile and can exceed 50 MPa in magnitude, a value high enough to deform copper, is reported. These stresses provide a significant driving force for fracture. Films are shown to be more unstable under tensile stress—and conversely more stable under compressive stress—when exposed to heat or humidity. Increasing the formation temperature of perovskite films directly correlates with larger residual stresses, a result of the high thermal expansion coefficient of perovskites. Specifically, this tensile stress forms upon cooling to room temperature, as the substrate constrains the perovskite from shrinking. No evidence of stress relaxation is observed, with the purely elastic film stress attributed to the thermal expansion mismatch between the perovskite and substrate. Additionally, the authors demonstrate that using a bath conversion method to form the perovskite film at room temperature leads to low stress values that are unaffected by further annealing, indicating complete perovskite formation prior to annealing. It is concluded that reducing the film stress is a novel method for improving perovskite stability, which can be accomplished by lower formation temperatures, flexible substrates with high thermal expansion coefficients, and externally applied compressive stress after fabrication.

Perovskite solar cells retain their performance with temperature cycling using a compliant, ethylene vinyl acetate encapsulant.

Significant effort has focused on controlling the deposition of perovskite films to enable uniform films, enabling efficiencies to climb dramatically. However, little attention has been paid to the evolution of thin-film stresses during deposition and the consequent effect on film morphology. While a textured surface topology has potential benefits for light scattering, a smooth surface is desirable to enable the pinhole-free deposition of contact layers. We show that the highly textured morphology made by popular antisolvent conversion methods arises because of in-plane compressive stress experienced during the intermediate phase of film formation where the substrate constrains the film from expanding—leading to energy release in the form of wrinkling, resulting in trenches that can be hundreds of nanometers deep with periods of several micrometers. We demonstrate that the extent of wrinkling is correlated with the rate of film conversion and that ultrasmooth films are obtained by slowing the rate of film formation.