Microscopic
understanding of interaction between H2O
and MAPbI3 (CH3NH3PbI3) is essential to further improve efficiency and stability of perovskite
solar cells. A complete picture of perovskite from initial physical
uptake of water molecules to final chemical transition to its monohydrate
MAPbI3·H2O is obtained with in situ infrared
spectroscopy, mass monitoring, and X-ray diffraction. Despite strong
affinity of MA to water, MAPbI3 absorbs almost no water
from ambient air. Water molecules penetrate the perovskite lattice
and share the space with MA up to one H2O per MA at high-humidity
levels. However, the interaction between MA and H2O through
hydrogen bonding is not established until the phase transition to
monohydrate where H2O and MA are locked to each other.
This lack of interaction in water-infiltrated perovskite is a result
of dynamic orientational disorder imposed by tetragonal lattice symmetry.
The apparent inertness of H2O along with high stability
of perovskite in an ambient environment provides a solid foundation
for its long-term application in solar cells and optoelectronic devices.
Organometal trihalide perovskites (OTP) have attracted significant attention as a low-cost and high-efficiency solar cell material. Due to the strong coordination between lead iodide (PbI2) and dimethyl sulfoxide (DMSO) solvent, a non-stoichiometric intermediate phase of MA2Pb3I8(DMSO)2 (MA = CH3NH3(+)) usually forms in the one-step deposition method that plays a critical role in attaining high power conversion efficiency. However, the kinetic understanding of how the non-stoichiometric intermediate phase transforms during thermal annealing is currently absent. In this work, we investigated such a phase transformation and provided a clear picture of three phase transition pathways as a function of annealing conditions. The interdiffusion of MAI and DMSO varies strongly with the annealing temperature and time, thus determining the final film composition and morphology. A surprising finding reveals that the best performing cells contain ∼18% of the non-stoichiometric intermediate phase, instead of pure phase OTP. The presence of such an intermediate phase enables smooth surface morphology and enhances the charge carrier lifetime. Our results highlight the importance of the intermediate phase growth kinetics that could lead to large-scale production of efficient solution processed perovskite solar cells.
High-quality perovskite light harvesters and robust organic hole extraction layers are essential for achieving high-performing perovskite solar cells (PSCs). We introduce a phosphonic acid–functionalized fullerene derivative in mixed-cation perovskites as a grain boundary modulator to consolidate the crystal structure, which enhances the tolerance of the film against illumination, heat, and moisture. We also developed a redox-active radical polymer, poly(oxoammonium salt), that can effectively p-dope the hole-transporting material by hole injection and that also mitigates lithium ion diffusion. Power conversion efficiencies of 23.5% for 1-square-centimeter mixed–cation-anion PSCs and 21.4% for 17.1-square-centimeter minimodules were achieved. The PSCs retained 95.5% of their initial efficiencies after 3265 hours at maximum power point tracking under continuous 1-sun illumination at 70° ± 5°C.
The phase of perovskite evolves when the non-stoichiometric mixed halide precursor is baked at different temperatures. Nb-doped TiO2nanorods are superior to plain nanorods as electron transport medium in crystallized perovskite.
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