Abstract The combined effects of compact TiO2(c‐TiO2) electron‐transport layer (ETL) are investigated without and with mesoscopic TiO2(m‐TiO2) on top, and without and with an iodine‐terminated silane self‐assembled monolayer (SAM), on the mechanical behavior, opto–electronic properties, photovoltaic (PV) performance, and operational‐stability of solar cells based on metal‐halide perovskites (MHPs). The interfacial toughness increases almost threefold in going from c‐TiO2without SAM to m‐TiO2with SAM. This is attributed to the synergistic effect of the m‐TiO2/MHP nanocomposite at the interface and the enhanced adhesion afforded by the iodine‐terminated silane SAM. The combination of m‐TiO2and SAM also offers a significant beneficial effect on the photocarriers extraction at the ETL/MHP interface, resulting in perovskite solar cells (PSCs) with power‐conversion efficiency (PCE) of over 24% and 20% for 0.1 and 1 cm2active areas, respectively. These PSCs also have exceptionally long operational‐stability lives: extrapolatedT80 (duration at 80% initial PCE retained) is ≈18 000 and 10 000 h for 0.1 and 1 cm2active areas, respectively.Postmortemcharacterization and analyses of the operational‐stability‐tested PSCs are performed to elucidate the possible mechanisms responsible for the long operational‐stability. 
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                            Interfacial toughening with self-assembled monolayers enhances perovskite solar cell reliability
                        
                    
    
            Iodine-terminated self-assembled monolayer (I-SAM) was used in perovskite solar cells (PSCs) to achieve a 50% increase of adhesion toughness at the interface between the electron transport layer (ETL) and the halide perovskite thin film to enhance mechanical reliability. Treatment with I-SAM also increased the power conversion efficiency from 20.2% to 21.4%, reduced hysteresis, and improved operational stability with a projected T80 (time to 80% initial efficiency retained) increasing from ~700 hours to 4000 hours under 1-sun illumination and with continuous maximum power point tracking. Operational stability–tested PSC without SAMs revealed extensive irreversible morphological degradation at the ETL/perovskite interface, including voids formation and delamination, whereas PSCs with I-SAM exhibited minimal damage accumulation. This difference was attributed to a combination of a decrease in hydroxyl groups at the interface and the higher interfacial toughness. 
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                            - Award ID(s):
- 2002158
- PAR ID:
- 10226666
- Publisher / Repository:
- American Association for the Advancement of Science (AAAS)
- Date Published:
- Journal Name:
- Science
- Volume:
- 372
- Issue:
- 6542
- ISSN:
- 0036-8075
- Page Range / eLocation ID:
- p. 618-622
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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