Behind the Scenes: Insights into the Structural Properties of Amide-Based Hole-Transporting Materials for Lead-Free Perovskite Solar Cells
Florian Wolf a, Maximilian Sirtl a, Sebastian Klenk a, Maximilian Wurzenberger a, Melina Armer b, Patrick Dörflinger b, Patrick Ganswindt a, Roman Guntermann a, Vladimir Dyakonov b, Thomas Bein a
a Department of Chemistry and Center for NanoScience (CeNS), University of Munich (LMU), Butenandtstrasse 5-13, D-81377 Munich, Germany
b Experimental Physics VI, Julius Maximilian University of Würzburg, 97074 Würzburg, Germany
International Conference on Hybrid and Organic Photovoltaics
Proceedings of International Conference on Hybrid and Organic Photovoltaics (HOPV23)
London, United Kingdom, 2023 June 12th - 14th
Organizers: Tracey Clarke, James Durrant and Trystan Watson
Oral, Florian Wolf, presentation 121
DOI: https://doi.org/10.29363/nanoge.hopv.2023.121
Publication date: 30th March 2023

Since lead-based perovskite solar cells still suffer several drawbacks such as a rather low stability against ambient conditions and severe toxicity of lead, lead-free double perovskite have emerged as new potential light-absorbing materials for solar cell applications. Among these materials, Cs2AgBiBr6 has so far been realized in solar cells exceeding a power conversion efficiency of 3 %.[1] To further optimize the solar cell performance, research focuses not only on the absorbing material itself but also on improving the charge-carrier transporting layers.[2] State-of-the-art perovskite solar cells often employ expensive organic hole transporting materials (HTM) such as Spiro-OMeTAD, motivating the search for more economical and better performing alternative HTMs.

Herein we report the crystal structure of EDOT-Amide-TPA from single crystal measurements as well as the first utilization of EDOT-Amide-TPA as a low-cost alternative to Spiro-OMeTAD as HTM in lead-free perovskite solar cells and link its stuctural properties to its superior charge carrier properties. It crystallizes in the triclinic space group P−1 with short intermolecular distances and very dense molecular packing, in contrast to the well-established HTM Spiro-OMeTAD. A comparison of EDOT-Amide-TPA with Spiro-OMeTAD shows an improved efficiency with the former when employed in lead-free double perovskite solar cells. Interestingly, in contrast to lead-based perovskites,[3] the better performance of EDOT-Amide-TPA cannot be attributed to higher VOC-values but rather to an improved charge carrier extraction, leading to higher JSC-values. This is confirmed by PL and EQE measurements and was explained by decreased recombination losses in the lead-free perovskite solar cells compared to the lead-based perovskites. The improved current densities were explained by the rather thin and compact HTM layer that is sufficient for EDOT-Amide-TPA, which is in line with the dense molecular packing in the solid state achieved by EDOT-Amide-TPA. The dense molecular packing of the HTM not only enables the formation of a thinner HTM layer but also increases the reproducibility of solar cell manufacturing.

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