Chloride-Based Additive Engineering for Efficient and Stable Wide-Bandgap Perovskite Solar Cells

Xinyi Shen; Benjamin M Gallant; Philippe Holzhey; Joel A Smith; Karim A Elmestekawy; Zhongcheng Yuan; P V G M Rathnayake; Stefano Bernardi; Akash Dasgupta; Ernestas Kasparavicius; Tadas Malinauskas; Pietro Caprioglio; Oleksandra Shargaieva; Yen-Hung Lin; Melissa M McCarthy; Eva Unger; Vytautas Getautis; Asaph Widmer-Cooper; Laura M Herz; Henry J Snaith

doi:10.1002/adma.202211742

Chloride-Based Additive Engineering for Efficient and Stable Wide-Bandgap Perovskite Solar Cells

Adv Mater. 2023 Jul;35(30):e2211742. doi: 10.1002/adma.202211742. Epub 2023 Jun 7.

Authors

Xinyi Shen¹, Benjamin M Gallant¹, Philippe Holzhey¹, Joel A Smith¹, Karim A Elmestekawy¹, Zhongcheng Yuan¹, P V G M Rathnayake², Stefano Bernardi², Akash Dasgupta¹, Ernestas Kasparavicius³, Tadas Malinauskas⁴, Pietro Caprioglio¹, Oleksandra Shargaieva⁵, Yen-Hung Lin¹, Melissa M McCarthy¹, Eva Unger^{5

6}, Vytautas Getautis⁴, Asaph Widmer-Cooper^{2

7}, Laura M Herz^{1

8}, Henry J Snaith¹

Affiliations

¹ Clarendon Laboratory, Department of Physics, University of Oxford, Parks Road, Oxford, OX1 3PU, UK.
² ARC Centre of Excellence in Exciton Science, School of Chemistry, University of Sydney, Sydney, NSW, 2006, Australia.
³ Department of Molecular Compound Physics, Centre for Physical Sciences and Technology, Sauletekio Avenue 3, Vilnius, LT-10257, Lithuania.
⁴ Department of Organic Chemistry, Kaunas University of Technology, Kaunas, LT-50254, Lithuania.
⁵ Young Investigator Group Hybrid Materials Formation and Scaling, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, D-14109, Berlin, Germany.
⁶ Chemical Physics and NanoLund, Lund University, Naturvetarvägen 14, Lund, 22362, Sweden.
⁷ The University of Sydney Nano Institute, University of Sydney, Sydney, NSW, 2006, Australia.
⁸ Institute for Advanced Study, TU Munich, Lichtenbergstr. 2a, D-85748, Garching, Germany.

PMID: 37191054
DOI: 10.1002/adma.202211742

Abstract

Metal halide perovskite based tandem solar cells are promising to achieve power conversion efficiency beyond the theoretical limit of their single-junction counterparts. However, overcoming the significant open-circuit voltage deficit present in wide-bandgap perovskite solar cells remains a major hurdle for realizing efficient and stable perovskite tandem cells. Here, a holistic approach to overcoming challenges in 1.8 eV perovskite solar cells is reported by engineering the perovskite crystallization pathway by means of chloride additives. In conjunction with employing a self-assembled monolayer as the hole-transport layer, an open-circuit voltage of 1.25 V and a power conversion efficiency of 17.0% are achieved. The key role of methylammonium chloride addition is elucidated in facilitating the growth of a chloride-rich intermediate phase that directs crystallization of the desired cubic perovskite phase and induces more effective halide homogenization. The as-formed 1.8 eV perovskite demonstrates suppressed halide segregation and improved optoelectronic properties.

Keywords: additive engineering; crystallization mechanism; halide homogenization; perovskite solar cells; suppressed halide segregation.

Abstract

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