More is Different: Mobile Ions Improve the Design Tolerances of Perovskite Solar Cells
Fraser J. Angus a, Lucy J. F. Hart b c, Yin Li d, Abdul Khaleed d, Philip Calado e, James R. Durrant c f, Aleksandra B. Djurišić d, Pablo Docampo a, Piers R. F. Barnes b
a University of Glasgow School of Chemistry Joseph Black Building Glasgow, G128QQ, UK
b Dept. of Physics and Centre for Processable Electronics, Imperial College London, London, SW7 2AZ, UK
c Department of Chemistry and Centre for Processable Electronics, Imperial College London, London, London W12 0BZ, United Kingdom
d Department of Physics, The University of Hong Kong, Hong Kong
e Department of Engineering, The Open University, Walton Hall, Milton Keynes, UK
f SPECIFIC IKC, Faculty of Science and Engineering, Swansea University, United Kingdom
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV25)
Roma, Italy, 2025 May 12th - 14th
Organizers: Filippo De Angelis, Francesca Brunetti and Claudia Barolo
Oral, Fraser J. Angus, presentation 095
Publication date: 17th February 2025

Do mobile ions help or hinder performance? Mobile halide ions in perovskite solar cells (PSCs) are often linked to negative effects such as degradation and hysteresis. However, this study demonstrates that mobile ions alter photovoltaic design parameters, enabling devices with mobile ions to achieve higher maximum efficiencies than those without.

Recent advancements in PSCs have been driven by surface treatments that reduce recombination and enhance photovoltages. These photovoltages often exceed the cells’ built-in potentials, with significant energetic offsets reported between the band edges of the perovskite and transport layers. This contradicts conventional photovoltaic design principles. This work attributes such tolerance for energetic offsets to mixed ionic and electronic conduction within the perovskite layer. Using the novel Stabilise and Pulse (SaP) technique, combined with drift-diffusion simulations, we explore how ionic charge distribution impacts performance. At steady-state, electrostatic redistribution of ions significantly reduces surface recombination currents, increasing photovoltage by tens to hundreds of millivolts. These findings reveal that mobile ions reduce the sensitivity of photovoltage to energetic misalignments at interfaces, ultimately improving device efficiency.

Building on these insights, we outline photovoltaic design principles that account for the effects of mobile ions and highlight the SaP method's capability to measure band offsets across different transport layers. These findings provide a new framework for optimising PSC design and performance.

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