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On the VOC loss in NiO-based inverted metal halide perovskite solar cells

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Abstract

Recent reports have shown that nickel oxide (NiO) when adopted as a hole transport layer (HTL) in combination with organic layers, such as PTAA or self-assembled monolayers (SAMs), leads to a higher device yield for both single junction as well as tandem devices. Nevertheless, implementing NiO in devices without PTAA or SAM is seldom reported to lead to high-performance devices. In this work, we assess the effect of key NiO properties deemed relevant in literature, namely- resistivity and surface energy, on the device performance and systematically compare the NiO-based devices with those based on PTAA. To this purpose, (thermal) atomic layer deposited (ALD) NiO (NiOBu-MeAMD), Al-doped NiO (Al:NiOBu-MeAMD), and plasma-assisted ALD NiO (NiOMeCp) films, characterized by a wide range of resistivity, are investigated. Although Al:NiOBu-MeAMD (∼400 Ω cm) and NiOMeCp(∼80 Ωcm) films have a lower resistivity than NiOBu-MeAMD (∼10 kΩ cm), the Al:NiOBu-MeAMD and NiOMeCp-based devices are found to have a modest open circuit voltage (VOC) gain of ∼30 mV compared to NiOBu-MeAMD-based devices. Overall, the best-performing NiO-based devices (∼14.8% power conversion efficiency (PCE)) still lag behind the PTAA-based devices (∼17.5%), primarily due to a VOC loss of ∼100 mV. Further investigation based on light intensity analysis of the VOC and FF and the decrease in VOC compared to the quasi-Fermi level splitting (QFLS) indicates that the VOC is limited by trap-assisted recombination at the NiO/perovskite interface. Additionally, SCAPS simulations show that the presence of a high interfacial trap density leads to a VOC loss in NiO-based devices. Upon passivation of the NiO/perovskite interface with Me-4PACz, the VOC increases by 170–200 mV and is similar for NiOBu-MeAMD and Al:NiOBu-MeAMD, leading to the conclusion that there is no influence of the NiO resistivity on the VOC once interface passivation is realized. Finally, our work highlights the necessity of comparing NiO-based devices with state-of-the-art HTL-based devices to draw conclusion about the influence of specific material properties on device performance.
Original languageEnglish
Pages (from-to)8652-8664
Number of pages13
JournalMaterials Advances
Volume5
Issue number21
Early online date14 Oct 2024
DOIs
Publication statusPublished - 7 Nov 2024

Funding

This work is carried out under the \u201CNew Energy and Mobility Outlook for the Netherlands\u201D (NEON) project with project number 17628 of the research programme NWO Crossover which is (partly) financed by the Dutch Research Council (NWO). The authors would like to thank Dr Christ H.L. Weijtens for carrying out the UPS measurements, Wim Arnold Bik (from Detect 99) for carrying out the RBS measurement at DIFFER and Caspar O. van Bommel, Joris J. I. M. Meulendijks, and Janneke J. A. Zeebregts for their technical support. K. M. acknowledges Wouter Vereijssen for his contribution to the surface energy studies and Marvin van Tilburg for his support during the PL measurements. K. M. thanks Dr Sinclair Ryley Ratnasingham for his insightful comments and help in the SCAPS simulation. M. C. acknowledges the NWO Aspasia program. V. Z. acknowledges the Research and Cooperation Fund from the Ministry of Economic Affairs and Climate Policy.

Funders
Nederlandse Organisatie voor Wetenschappelijk Onderzoek
Ministerie van Economische Zaken en Klimaat

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