Publication date: 17th February 2025
Wide-bandgap (WBG) perovskites are essential for tandem solar cells but often suffer from voltage deficits due to nonradiative recombination and halide segregation. Although rubidium (Rb+) incorporation has improved crystallinity and stability in single-junction devices, its integration into perovskite lattices usually leads to non-perovskite phase. Here, we demonstrate a strain-stabilized strategy enabling effective Rb+ incorporation into triple-halide perovskite lattices. By co-introducing chloride and leveraging lattice strain, the ionic size mismatch is compensated, suppressing phase segregation and ensuring homogeneous ion distribution across the film thickness.
The resulting WBG perovskite (bandgap: 1.67 eV) exhibits a photoluminescence quantum yield (PLQY) exceeding 14% and a quasi–Fermi level splitting of ~1.34 V and. A corresponding solar cell achieves a stabilized open-circuit voltage (VOC) of 1.30 V—93.5% of its radiative limit. This represents the lowest photovoltage loss reported for perovskites of bandgap ≥1.62 eV. Structural analyses (XRD, GIWAXS), compositional depth profiling (XPS), and spectroscopic measurements (PL, TRPL) reveal lattice homogenization, enlarged grain domain size, and suppressed nonradiative recombination. In-situ temperature-dependent XRD and theoretical calculation further confirm that Rb+ incorporation favorable only in the presence of both strain and chloride.
Our results establish a generalizable route for stabilizing metastable cations in perovskite lattices through cooperative lattice engineering. This approach not only unlocks new opportunities for high-efficiency tandem photovoltaics but also deepens the understanding of strain in compositional engineering of metal halide perovskites.
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