Journal
ADVANCED MATERIALS
Volume 32, Issue 42, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202004630
Keywords
crystallization kinetics; perovskite solar cells; reaction enthalpy; sequential A-site doping; two-step method
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Funding
- Research Grant Council of Hong Kong (RGC) [14314216]
- China Scholarship Council (CSC)
- Computational Sciences for Energy Research (CSER) tenure track program of Shell
- NWO, The Netherlands [15CST04-2]
- RGC (CRF Group Research Grant) [C5037-18G]
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Two-step-fabricated FAPbI(3)-based perovskites have attracted increasing attention because of their excellent film quality and reproducibility. However, the underlying film formation mechanism remains mysterious. Here, the crystallization kinetics of a benchmark FAPbI(3)-based perovskite film with sequential A-site doping of Cs(+)and GA(+)is revealed by in situ X-ray scattering and first-principles calculations. Incorporating Cs(+)in the first step induces an alternative pathway from delta-CsPbI(3)to perovskite alpha-phase, which is energetically more favorable than the conventional pathways from PbI2. However, pinholes are formed due to the nonuniform nucleation with sparse delta-CsPbI(3)crystals. Fortunately, incorporating GA(+)in the second step can not only promote the phase transition from delta-CsPbI(3)to the perovskite alpha-phase, but also eliminate pinholes via Ostwald ripening and enhanced grain boundary migration, thus boosting efficiencies of perovskite solar cells over 23%. This work demonstrates the unprecedented advantage of the two-step process over the one-step process, allowing a precise control of the perovskite crystallization kinetics by decoupling the crystal nucleation and growth process.
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