Crystal Growth Modulation of Tin-Lead Halide Perovskites via Chaotropic Agent
Thomas J. Macdonald a
a Department of Electronic & Electrical Engineering, Roberts Building, University College London
NIPHO25
Proceedings of International Conference on Perovskite Thin Film Photovoltaics and Perovskite Photonics and Optoelectronics (NIPHO25)
Cagliari, Italy, 2025 June 9th - 10th
Organizers: Giulia Grancini, Daniela Marongiu and Aldo Di Carlo
Oral, Thomas J. Macdonald, presentation 037
Publication date: 24th April 2025

Mixed tin-lead (Sn-Pb) halide perovskites, with their tuneable bandgaps (1.2–1.4 eV), show great promise for the development of highly efficient all-perovskite tandem solar cells. However, achieving commercial viability and stabilized high efficiency for Sn-Pb perovskite solar cells (PSCs) presents numerous challenges.  Among various optimization strategies, incorporating additives has proven critical in modulating the crystallization of Sn-Pb halide perovskites. Despite the widespread use of additives to improve performance, the detailed photophysical mechanisms remain unclear. In this work, we elucidate the mechanistic role of guanidinium thiocyanate, a chaotropic agent, in the crystallization of Sn-Pb halide perovskites. We combine hyperspectral imaging with real-time in-situ photoluminescence spectroscopy, to study the crystallization process of Sn-Pb halide perovskites. Our findings reveal that the chaotropic agent modulates the crystal growth rate during perovskite crystallization, resulting in more homogeneous films with reduced non-radiative recombination. We challenge the common assumption that crystallization stops once the solvent evaporates by identifying photoluminescence variations during the cooldown process. The resulting films exhibit a photoluminescence quantum yield of 7.28% and a charge carrier lifetime exceeding 11 µs, leading to a device efficiency of 22.34% and a fill factor of over 80%. This work provides a fundamental understanding of additive-mediated crystal growth and transient cooldown dynamics, advancing the design of high-quality Sn-Pb perovskites for efficient and stable optoelectronics.

 

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