Electrostatically Enhanced Buried Interface Binding of Self‐Assembled Monolayers for Efficient And Stable Inverted Perovskite Solar Cells

Inverted p-i-n structure perovskite solar cells (PSCs) have outperformed traditional n-i-p PSCs in recent years. A key advancement is the use of self-assembled monolayers (SAMs) as hole transport layers. One class of widely used SAMs is carbazole-based phosphonic acids. However, it is found that these SAMs lack strong binding with transparent conducting oxides (TCO) and perovskite. The weak binding strength results in suboptimal interfacial adhesion of the buried interface, which limits the device's stability. Here, interfacial binding is enhanced by increasing the dipole moment that creates a strong interfacial electric field that enhances electrostatic interactions at the TCO/perovskite interface, while incorporating tailored functional groups in SAMs to improve chemical anchoring to TCO and binding to perovskite. Specifically, the donor-acceptor SAM molecule 4-(7-(4-(bis(4-methoxyphenyl)amino)-2,5-difluorophenyl)benzo[c][1,2,5]thiadiazol-4-yl)benzoic acid (PAFTB) is employed, which features an enhanced dipole moment along with electron-donating and electron-withdrawing functional groups to optimize interfacial interactions. Compared to extensively used [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz), PAFTB enhances total interfacial adhesion by 2.8 times, thereby improving the thermal stability of the layer. Using this approach, PSCs are demonstrated with a certified quasi-steady-state power conversion efficiency of 24.9% and maintain 80% of the initial efficiency after 900 h of maximum power point tracking at 85 °C.

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Publication Details

Journal
Advanced Materials
Published
2025-08-11
DOI
https://doi.org/10.1002/adma.202508740
Citations
10
Primary Topic
Perovskite Materials and Applications
Type
article
Field-Weighted Citation Impact
7.30

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Electrostatically Enhanced Buried Interface Binding of Self‐Assembled Monolayers for Efficient And Stable Inverted Perovskite Solar Cells

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10 citations
Advanced Materials
Perovskite Materials and Applications
7.30
article

Electrostatically Enhanced Buried Interface Binding of Self‐Assembled Monolayers for Efficient And Stable Inverted Perovskite Solar Cells

Isaiah W. Gilley, Abdulaziz S. R. Bati, Lin X. Chen, Chuying Huang, Mercouri G. Kanatzidis, Cheng Liu, Nicholas Rolston, Edward Hartley Sargent, George Chappell Schatz, Subhajyoti Chaudhuri, Tobin Filleter, Yi Yang, Peter Serles, Boran Kumral, Woo Cheol Jeon, Hao Chen, Bin Chen, Muzhi Li
article en
10 citations

Abstract

Inverted p-i-n structure perovskite solar cells (PSCs) have outperformed traditional n-i-p PSCs in recent years. A key advancement is the use of self-assembled monolayers (SAMs) as hole transport layers. One class of widely used SAMs is carbazole-based phosphonic acids. However, it is found that these SAMs lack strong binding with transparent conducting oxides (TCO) and perovskite. The weak binding strength results in suboptimal interfacial adhesion of the buried interface, which limits the device's stability. Here, interfacial binding is enhanced by increasing the dipole moment that creates a strong interfacial electric field that enhances electrostatic interactions at the TCO/perovskite interface, while incorporating tailored functional groups in SAMs to improve chemical anchoring to TCO and binding to perovskite. Specifically, the donor-acceptor SAM molecule 4-(7-(4-(bis(4-methoxyphenyl)amino)-2,5-difluorophenyl)benzo[c][1,2,5]thiadiazol-4-yl)benzoic acid (PAFTB) is employed, which features an enhanced dipole moment along with electron-donating and electron-withdrawing functional groups to optimize interfacial interactions. Compared to extensively used [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2PACz), PAFTB enhances total interfacial adhesion by 2.8 times, thereby improving the thermal stability of the layer. Using this approach, PSCs are demonstrated with a certified quasi-steady-state power conversion efficiency of 24.9% and maintain 80% of the initial efficiency after 900 h of maximum power point tracking at 85 °C.

Advanced MaterialsVol. 37(43)
Northwestern University (US), University of Toronto (CA), Arizona State University (US)
National Science Foundation, U.S. Department of Energy, Northwestern University, King Abdullah University of Science and Technology, Office of Science, Office of Energy Efficiency and Renewable Energy, Materials Research Science and Engineering Center, Harvard University, International Institute for Nanotechnology, Northwestern University, Division of Materials Research, Division of Electrical, Communications and Cyber Systems, Division of Chemistry, Basic Energy Sciences, Solar Energy Technologies Office, Office of Energy Efficiency, Argonne National Laboratory
Affordable and clean energy
Openalex Percentile: Top 3%
Perovskite Materials and Applications
7.30
DOIOpen Access PDFOpenAlex
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