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[ASAP] Phase-Pure Hybrid Layered Lead Iodide Perovskite Films Based on a Two-Step Melt-Processing Approach
Efficient composition tuning via cation exchange and improved reproducibility of photovoltaic performance in FAxMA1-xPbI3 planar heterojunction solar cells fabricated by a two-step dynamic spin-coating process
Publication date: December 2018
Source: Nano Energy, Volume 54
Author(s): Kyungeun Jung, Jae-Ho Lee, Kwonwoo Oh, Chan Im, Junghwan Do, Joosun Kim, Weon-Sik Chae, Man-Jong Lee
Abstract
We synthesized uniform FAxMA1-xPbI3 perovskite films with a single α phase by a two-step process combined with a dynamically dispensed spin-coating technique. It uses the continuous dropping of precursor solutions with a constant CH3NH3I (MAI)/HC(NH2)2I (FAI) concentration enabling the kinetically controlled grain growth. Dynamic coating cycles are also changed to facilitate a cation-exchange process, control the degree of the mutual inter-mixing between formamidinium lead triiodide (FAPbI3) and methylammonium lead triiodide (MAPbI3) and examine the formation process and properties of the mixed perovskite films formed under the excess MA/FA cation environment, which has not been clarified so far. Notably, without additional solvent washing steps, FAxMA1-xPbI3 films are adjustable in composition, pinhole-free, and have various grain sizes depending on the coating cycles. Perovskite solar cells (PSCs) synthesized from FAxMA1-xPbI3 films with two cycles of the dynamic spin coating have achieved a maximum power conversion efficiency (PCE) of 18.50% with an average PCE of 17.06 ± 0.42%, which shows much-improved performance as well as reproducibility compared with 14.79 ± 1.82% obtained from the conventional static spin-coating method. In addition, we first found mixed FAxMA1-xPbI3 perovskites synthesized under an excess cation environment containing local stoichiometric inhomogeneities as well as excess residual cations (C˭N and NH3+) acting as recombination traps, which is supported by the calculation of trap densities.
Graphical abstract

Hierarchical SnO2 Nanostructures: Recent Advances in Design, Synthesis, and Applications
Enhanced optical output in InGaN/GaN light-emitting diodes by tailored refractive index of nanoporous GaN
Enhanced stability of the optical responses from all-inorganic perovskite nanocrystals embedded in a synthetic opal matrix
[ASAP] Controlling Solvate Intermediate Growth for Phase-Pure Organic Lead Iodide Ruddlesden–Popper (C4H9NH3)2(CH3NH3)n-1PbnI3n+1 Perovskite Thin Films
[ASAP] Improving the Photovoltaic Performance and Mechanical Stability of Flexible All-Polymer Solar Cells via Tailoring Intermolecular Interactions
[ASAP] Asymmetric 3D Hole-Transporting Materials Based on Triphenylethylene for Perovskite Solar Cells
[ASAP] Constructing Gradient Energy Levels to Promote Exciton Energy Transfer for Photoluminescence Controllability of All-Inorganic Perovskites and Application in Single-Component WLEDs
[ASAP] High-throughput Computational Study of Halide Double Perovskite Inorganic Compounds
[ASAP] Ternary Phase Diagram-Facilitated Rapid Screening of Double Perovskites As Electrocatalysts for the Oxygen Evolution Reaction
High‐Pressure Band‐Gap Engineering and Metallization in the Perovskite Derivative Cs3Sb2I9
Under pressure: Cs3Sb2I9 undergoes large‐scale band‐gap narrowing, reversible amorphization, and piezochromism under high pressure. The narrow band gap of Cs3Sb2I9 at the highest pressure satisfies the optimal band‐gap requirement of the Shockley–Queisser limit. The sample exhibits metallic conductor properties at 44.3 GPa, revealing a wholly new electronic landscape and transport properties.
Abstract
Among photovoltaic materials, the antimony‐based, perovskite‐like structure Cs3Sb2I9 stands out owing to its low toxicity and air stability. Here, changes in the optoelectronic properties and crystal structure of the lead‐free perovskite derivative Cs3Sb2I9 are reported, caused by pressure‐induced lattice compression. At 20.0 GPa, Cs3Sb2I9 with a wide band gap (2.34 eV) successfully broke through the Shockley–Queisser limit (1.34 eV), accompanied by clear piezochromism from orange–yellow to opaque black. Additionally, Cs3Sb2I9 experienced completely reversible amorphization at 20.0 GPa. These optical changes could be attributed to atomic‐orbital overlap enhancement caused by contraction of the Sb−I bond length and diminution of the Sb−I bond angle. In addition, Cs3Sb2I9 underwent a transition from semiconductor to conductor upon compression and obtained metallic properties at 44.3 GPa, indicating new electronic properties. The obtained results may further broaden the research prospects of halide perovskite materials in the field of photovoltaics.






