Prof Henry Snaith FRS

Abstract:

Mixed halide perovskites exhibit promising optoelectronic properties for next-generation light-emitting diodes due to their tunable emission wavelength that covers the entire visible light spectrum. However, these materials suffer from severe phase segregation under continuous illumination, making long-term stability for pure red emission a significant challenge. In this study, we present a comprehensive analysis of the role of halide oxidation in unbalanced ion migration (I/Br) within CsPbI₂Br nanocrystals and thin films. We also introduce a new approach using cyclic olefin copolymer (COC) to encapsulate CsPbI₂Br perovskite nanocrystals (PNCs), effectively suppressing ion migration by increasing the corresponding activation energy. Compared with that of unencapsulated samples, we observe a substantial reduction in phase separation under intense illumination in PNCs with a COC coating. Our findings show that COC enhances phase stability by passivating uncoordinated surface defects (Pb²⁺ and I^-), increasing the formation energy of halide vacancies, improving the charge carrier lifetime, and reducing the nonradiative recombination density.

Abstract:

While amines are widely used as additives in metal-halide perovskites, our understanding of the way amines in perovskite precursor solutions impact the resultant perovskite film is still limited. In this paper, we explore the multiple effects of benzylamine (BnAm), also referred to as phenylmethylamine, used to passivate both FA_0.75Cs_0.25Pb(I_0.8Br_0.2)₃ and FA_0.8Cs_0.2PbI₃ perovskite compositions. We show that, unlike benzylammonium (BnA⁺) halide salts, BnAm reacts rapidly with the formamidinium (FA⁺) cation, forming new chemical products in solution and these products passivate the perovskite crystal domains when processed into a thin film. In addition, when BnAm is used as a bulk additive, the average perovskite solar cell maximum power point tracked efficiency (for 30 s) increased to 19.3% compared to the control devices 16.8% for a 1.68 eV perovskite. Under combined full spectrum simulated sunlight and 65 °C temperature, the devices maintained a better T₈₀ stability of close to 2500 h while the control devices have T₈₀ stabilities of <100 h. We obtained similar results when presynthesizing the product BnFAI and adding it directly into the perovskite precursor solution. These findings highlight the mechanistic differences between amine and ammonium salt passivation, enabling the rational design of molecular strategies to improve the material quality and device performance of metal-halide perovskites.

Abstract:

Recently, there has been an extensive focus on inverted perovskite solar cells (PSCs) with a p-i-n architecture due to their attractive advantages, such as exceptional stability, high efficiency, low cost, low-temperature processing, and compatibility with tandem architectures, leading to a surge in their development. Single-junction and perovskite-silicon tandem solar cells (TSCs) with an inverted architecture have achieved certified PCEs of 26.15% and 33.9% respectively, showing great promise for commercial applications. To expedite real-world applications, it is crucial to investigate the key challenges for further performance enhancement. We first introduce representative methods, such as composition engineering, additive engineering, solvent engineering, processing engineering, innovation of charge transporting layers, and interface engineering, for fabricating high-efficiency and stable inverted PSCs. We then delve into the reasons behind the excellent stability of inverted PSCs. Subsequently, we review recent advances in TSCs with inverted PSCs, including perovskite-Si TSCs, all-perovskite TSCs, and perovskite-organic TSCs. To achieve final commercial deployment, we present efforts related to scaling up, harvesting indoor light, economic assessment, and reducing environmental impacts. Lastly, we discuss the potential and challenges of inverted PSCs in the future.