Beyond the Surface: Three-Dimensional Distribution and Defect Passivation of Self-Assembled Monolayers in Perovskite Solar Cells

Self-assembled monolayers (SAMs) are widely employed to tune interfacial properties in perovskite solar cells (PSCs), yet they have so far been regarded as strictly two-dimensional surface modifiers. Here, we uncover the three-dimensional (3D) nature of perfluorinated silanol-based SAMs applied onto perovskite films and their impact on both the photovoltaic performance and stability of PSCs. Using high-resolution 3D nanoscale secondary ion mass spectrometry, which directly maps their lateral and vertical distribution, we reveal that these SAMs not only decorate the perovskite surface but also selectively penetrate and anchor at grain-boundary iodine-deficient regions within ∼100 nm of the film. This dual surface-bulk passivation reshapes the defect landscape in perovskite thin films, yielding reduced nonradiative recombination, more favorable interfacial energetics, enhanced photovoltaic performance, and increased environmental stability. Our findings reposition SAMs as volumetric chemical modifiers rather than merely interface dipole layers, highlighting their potential for molecular-level engineering in perovskite optoelectronics.

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Publication Details

Journal
ACS Nano
Published
2026-03-31
DOI
https://doi.org/10.1021/acsnano.6c00728
Primary Topic
Perovskite Materials and Applications
Type
article
Field-Weighted Citation Impact
0.00

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article

Beyond the Surface: Three-Dimensional Distribution and Defect Passivation of Self-Assembled Monolayers in Perovskite Solar Cells

Lionel Aigouy, José Álvarez, Jiazhuo Nie, Sergio Vlaic et al.
ACS Nano
Perovskite Materials and Applications
article

Beyond the Surface: Three-Dimensional Distribution and Defect Passivation of Self-Assembled Monolayers in Perovskite Solar Cells

Lionel Aigouy, José Álvarez, Jiazhuo Nie, Sergio Vlaic, Philippe Lang, Dongjiu Zhang, Smail Mostefaoui, Daming Zheng, Thierry Pauporté, Jérôme Aléon, Yusheng Wang, Rebeca Lopez-Adams, Zhuoying Chen
article en

Abstract

Self-assembled monolayers (SAMs) are widely employed to tune interfacial properties in perovskite solar cells (PSCs), yet they have so far been regarded as strictly two-dimensional surface modifiers. Here, we uncover the three-dimensional (3D) nature of perfluorinated silanol-based SAMs applied onto perovskite films and their impact on both the photovoltaic performance and stability of PSCs. Using high-resolution 3D nanoscale secondary ion mass spectrometry, which directly maps their lateral and vertical distribution, we reveal that these SAMs not only decorate the perovskite surface but also selectively penetrate and anchor at grain-boundary iodine-deficient regions within ∼100 nm of the film. This dual surface-bulk passivation reshapes the defect landscape in perovskite thin films, yielding reduced nonradiative recombination, more favorable interfacial energetics, enhanced photovoltaic performance, and increased environmental stability. Our findings reposition SAMs as volumetric chemical modifiers rather than merely interface dipole layers, highlighting their potential for molecular-level engineering in perovskite optoelectronics.

ACS NanoVol. 20(14)
Macau University of Science and Technology (MO), Centre National de la Recherche Scientifique (FR), Université Paris Cité (FR), Université Paris Sciences et Lettres (FR), Université Paris-Saclay (FR), Laboratoire de Génie Électrique et Électronique de Paris (FR), Sorbonne Université (FR), Laboratoire de Physique et d’Étude des Matériaux (FR), Laboratoire de Minéralogie & Cosmochimie du Muséum (FR), Institute of Molecular Functional Materials (CN), CentraleSupélec (FR), Institut de Recherche de Chimie Paris (FR), Interfaces Traitements Organisation et Dynamique des Systèmes (FR), Division of Materials Science and Engineering (AU), Institut de minéralogie, de physique des matériaux et de cosmochimie (FR), Institut de Recherche pour le Développement (FR), ESPCI Paris (FR)
Agence Nationale de la Recherche, Ministry of Education of the People's Republic of China, Ministère de l'Europe et des Affaires Étrangères, China Scholarship Council, Ministère de l'Education Nationale, de l'Enseignement Superieur et de la Recherche
Openalex Percentile: Top 38%
Perovskite Materials and Applications
DOIOpen Access PDFOpenAlex
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