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Cations with suitable sizes to occupy an interstitial site of perovskite crystals have been widely used to inhibit ion migration and promote the performance and stability of perovskite optoelectronics. However, such interstitial doping inevitably leads to lattice microstrain that impairs the long-range ordering and stability of the crystals, causing a sacrificial trade-off. Here, we unravel the evident influence of the valence states of the interstitial cations on their efficacy to suppress the ion migration. Incorporation of a trivalent neodymium cation (Nd3+) effectively mitigates the ion migration in the perovskite lattice with a reduced dosage (0.08%) compared to a widely used monovalent cation dopant (Na+, 0.45%). The photovoltaic performances and operational stability of the prototypical perovskite solar cells are enhanced with a trace amount of Nd3+ doping while minimizing the sacrificial trade-off.

Optoelectronic devices consist of heterointerfaces formed between dissimilar semiconducting materials. The relative energy-level alignment between contacting semiconductors determinately affects the heterointerface charge injection and extraction dynamics. For perovskite solar cells (PSCs), the heterointerface between the top perovskite surface and a charge-transporting material is often treated for defect passivation(1-4) to improve the PSC stability and performance. However, such surface treatments can also affect the heterointerface energetics(1). Here we show that surface treatments may induce a negative work function shift (that is, more n-type), which activates halide migration to aggravate PSC instability. Therefore, despite the beneficial effects of surface passivation, this detrimental side effect limits the maximum stability improvement attainable for PSCs treated in this way. This trade-off between the beneficial and detrimental effects should guide further work on improving PSC stability via surface treatments.

Semi-transparent organic photovoltaics (OPVs) are an emerging solar-energy-harvesting technology with promising applications, such as rooftop energy supplies for environmentally friendly greenhouses. However, the poor operational stability of OPVs poses challenges to their feasibility as incessantly serving facilities. Here we report a reductive interlayer structure for semi-transparent OPVs that improves the operational stability of OPVs under continuous solar radiation. The interlayer effectively suppresses the generation of radicals from the electron transport layer under sunlight and prevents the structural decomposition of the organic photoactive layer during operation. The defects that serve as the charge carrier recombination sites are nullified by the electron-donating functional groups of the reduced molecules, which improves photovoltaic performance. The semi-transparent OPVs demonstrate a power conversion efficiency of 13.5% and an average visible transmittance of 21.5%, with remarkable operational stability (84.8% retention after 1,008 h) under continuous illumination. Greenhouse results show that the semi-transparent OPV roof benefits the survival rate and growth of the crops, indicating the importance of our approach in addressing food and energy challenges.