Vertically oriented low-dimensional perovskites for high-efficiency wide band gap perovskite solar cells

Andrea Zanetta, Valentina Larini, Vikram, Francesco Toniolo, Badri Vishal, Karim A. Elmestekawy, Jiaxing Du, Alice Scardina, Fabiola Faini, Giovanni Pica, Valentina Pirota, Matteo Pitaro, Sergio Marras, Changzeng Ding, Bumin K. Yildirim, Maxime Babics, Esma Ugur, Erkan Aydin, Chang-Qi Ma, Filippo Doria, Maria Antonietta Loi, Michele De Bastiani, Laura M. Herz, Giuseppe Portale, Stefaan De Wolf, M. Saiful Islam and Giulia Grancini ()
Additional contact information
Andrea Zanetta: Via T. Taramelli 14
Valentina Larini: Via T. Taramelli 14
Vikram: University of Oxford
Francesco Toniolo: Via T. Taramelli 14
Badri Vishal: Physical Sciences and Engineering Division (PSE)
Karim A. Elmestekawy: Clarendon Laboratory
Jiaxing Du: Clarendon Laboratory
Alice Scardina: Via T. Taramelli 14
Fabiola Faini: Via T. Taramelli 14
Giovanni Pica: Via T. Taramelli 14
Valentina Pirota: Via T. Taramelli 14
Matteo Pitaro: University of Groningen Nijenborgh 3 (Feringa Building)
Sergio Marras: Via Morego 30
Changzeng Ding: SIP
Bumin K. Yildirim: Physical Sciences and Engineering Division (PSE)
Maxime Babics: Physical Sciences and Engineering Division (PSE)
Esma Ugur: Physical Sciences and Engineering Division (PSE)
Erkan Aydin: Physical Sciences and Engineering Division (PSE)
Chang-Qi Ma: SIP
Filippo Doria: Via T. Taramelli 14
Maria Antonietta Loi: University of Groningen Nijenborgh 3 (Feringa Building)
Michele De Bastiani: Via T. Taramelli 14
Laura M. Herz: Clarendon Laboratory
Giuseppe Portale: University of Groningen Nijenborgh 3 (Feringa Building)
Stefaan De Wolf: Physical Sciences and Engineering Division (PSE)
M. Saiful Islam: University of Oxford
Giulia Grancini: Via T. Taramelli 14

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Controlling crystal growth alignment in low-dimensional perovskites (LDPs) for solar cells has been a persistent challenge, especially for low-n LDPs (n 1.7 eV) impeding charge flow. Here we overcome such transport limits by inducing vertical crystal growth through the addition of chlorine to the precursor solution. In contrast to 3D halide perovskites (APbX3), we find that Cl substitutes I in the equatorial position of the unit cell, inducing a vertical strain in the perovskite octahedra, and is critical for initiating vertical growth. Atomistic modelling demonstrates the thermodynamic stability and miscibility of Cl/I structures indicating the preferential arrangement for Cl-incorporation at I-sites. Vertical alignment persists at the solar cell level, giving rise to a record 9.4% power conversion efficiency with a 1.4 V open circuit voltage, the highest reported for a 2 eV wide band gap device. This study demonstrates an atomic-level understanding of crystal tunability in low-n LDPs and unlocks new device possibilities for smart solar facades and indoor energy generation.

Date: 2024
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DOI: 10.1038/s41467-024-53339-6

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