Publication date: 5th November 2025
Organic-inorganic halide perovskites have emerged as promising materials for next-generation optoelectronic devices due to their exceptional photophysical properties. Among them, α-formamidinium lead tri-iodide (α-FAPbI₃) with a cubic symmetry (space group of .) has garnered attention as a potential absorber in solar cells for its narrow bandgap and superior stability. However, the fundamental mechanisms underlying its high performance remain elusive. As recent studies reported incorporation of methylammonium chloride (MACl) to stabilize α-FAPbI3, herein, we propose that crystallization process of α-FAPbI3 can be kinetically controlled by adjusting MACl concentration. We examined higher concentration of MACl induces slower crystallization kinetics, resulting in larger grain size and [100] preferred orientation. In this presentation, centro-symmetry breaking in [001] preferred oriented α-FAPbI₃ thin films (POF) arises from inevitable anisotropic strain during film formation will be discussed. Using circular polarization-dependent pump-probe transient absorption (CPTA), we observe Rashba-type band splitting exclusively in POF, indicating symmetry breaking. Angle dependent X-ray diffraction and photoluminescence (PL) reveal significant residual stress in POF compared to randomly oriented films (ROF), confirming strain-induced lattice distortion. Furthermore, time-resolved PL (TRPL), and time-resolved microwave conductivity (TRMC) measurements reveal top-back inhomogeneous carrier dynamics and anisotropic charged carrier mobility, supporting the presence of strain-induced symmetry breaking. Furthermore, we present an amorphous TiO2 and V2O5-x passivation layers, deposited by atomic layer deposition (ALD) at low temperature (< 50 ℃), on Spiro-OMeTAD to prevent metal-induced interfacial degradation while maintaining the overall performance. Finally, we have fabricated perovskite solar cells (FTO/SnO2-based ALD-ETL/FAPbI3/2Dperovskite/Spiro-OMeTAD/Au) and confirmed increased PCE (23.91 %) measured under AM 1.5 G. Not only PCE, but also device stability with ALD-TiO2 and V2O5-x layers was dramatically improved. It was confirmed through ion contents profiling using ToF-SIMS that the improvement of the stability in PSC adopting ALD-TiO2 and V2O5-x comes from preventing the metal ion diffusion. In conclusion, we have demonstrated high PCE and stability of PSCs.
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