Foldable Hole‐Transporting Materials for Merging Electronic States between Defective and Perfect Perovskite Sites

• Published in: Advanced materials (Weinheim) Vol. 35; no. 25; pp. e2300720 - n/a
• Main Authors: Xia, Jianxing, Luizys, Povilas, Daskeviciene, Maryte, Xiao, Chuanxiao, Kantminiene, Kristina, Jankauskas, Vygintas, Rakstys, Kasparas, Kreiza, Gediminas, Gao, Xiao‐Xin, Kanda, Hiroyuki, Brooks, Keith Gregory, Alwani, Imanah Rafieh, Ain, Qurat Ul, Zou, Jihua, Shao, Guang, Hu, Ruiyuan, Qiu, Zeliang, Slonopas, Andre, Asiri, Abdullah M., Zhang, Yi, Dyson, Paul J., Getautis, Vytautas, Nazeeruddin, Mohammad Khaja
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 01.06.2023
• Subjects: Electron states; Energy conversion efficiency; hole mobility; hole‐transporting materials; Materials science; Modules; perovskite solar cells; Perovskites; photovoltaics; Transportation; trap states; Valence band; Wave functions; trap states; hole-transporting materials; hole mobility; perovskite solar cells; photovoltaics
• ISSN: 0935-9648; 1521-4095
• DOI: 10.1002/adma.202300720

Defective and perfect sites naturally exist within electronic semiconductors, and considerable efforts to reduce defects to improve the performance of electronic devices, especially in hybrid organic–inorganic perovskites (ABX3), are undertaken. Herein, foldable hole‐transporting materials (HTMs) are developed, and they extend the wavefunctions of A‐site cations of perovskite, which, as hybridized electronic states, link the trap states (defective site) and valence band edge (perfect site) between the naturally defective and perfect sites of the perovskite surface, finally converting the discrete trap states of the perovskite as the continuous valence band to reduce trap recombination. Tailoring the foldability of the HTMs tunes the wavefunctions between defective and perfect surface sites, allowing the power conversion efficiency of a small cell to reach 23.22% and that of a mini‐module (6.5 × 7 cm, active area = 30.24 cm2) to reach as high as 21.71% with a fill factor of 81%, the highest value reported for non‐spiro‐OMeTAD‐based perovskite solar modules. Merging orbitals between the defect and perfect crystals within perovskites are found in chemosynthetic foldable hole‐transporting materials (HTMs) that convert discrete island trap states to continuous electronic states, and the mini module achieves high efficiency and fill factor.