Publication date: 11th March 2026
Organic halide perovskites have achieved remarkable power conversion efficiencies, exceeding 35% in tandem and 27.3% in single-junction devices. However, long-term operational stability remains the primary barrier to commercialization. While macroscopic degradation trends are well documented and been presented at HOPV in Rome last year [1], the microscopic origins of instability and their relation to crystallographic structure are still insufficiently understood.
In this work, we combine macroscopic ageing studies with grain-resolved correlative atomic force microscopy and electron backscatter diffraction to investigate degradation in perovskite thin films under ambient conditions and illumination. Time-resolved AFM reveals heterogeneous surface evolution, ranging from intact grains to partially and fully degraded grains. Local RMS roughness analysis provides a quantitative measure of degradation onset and progression at the level of individual grains.
By correlating morphological changes with crystallographic orientation, we show that degradation is strongly orientation dependent. Grains oriented near {100} exhibit the fastest roughening, whereas grains oriented closer to {110} and {111} remain significantly more stable. Substrate-dependent experiments further demonstrate that interfacial properties and initial texture govern whether degradation occurs heterogeneously and slow, as on ITO, or more uniformly but considerably faster, as on glass and quartz.
These results provide direct microscopic evidence that crystallographic orientation controls the environmental stability of perovskite thin films. Suppressing the {100} texture and optimizing substrate interfaces emerge as a promising strategy to enhance the long-term operational stability of perovskite optoelectronic devices.
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