Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.
Advertisement
Nature Energy (2026)
Robust hole-selective interfaces are critical for the stability of perovskite solar cells, yet this requirement is inadequately addressed by self-assembled monolayers (SAMs). Here we combine (4-(7H-dibenzo[c,g]carbazol-7-yl)butyl)phosphonic acid (CbzNaph) and its hydroxyl functionalized analogue (CbzNaphOH), which features intramolecular hydrogen-bonding interactions between the spacer and anchoring groups, to modulate SAM molecular packing. Increased steric hindrance promotes the formation of an amorphous self-assembled multilayer (a-SAMUL) with homogeneous packing. This amorphous layer acts simultaneously as a uniform, strongly adhesive binding medium that tightly couples the perovskite and substrate—thereby suppressing the formation of mobile ions—and as an efficient hole-selective contact with favourable energy-level alignment. Devices incorporating a-SAMULs achieve a certified efficiency exceeding 26% and reduced ion-migration-driven degradation. The devices exhibit reverse breakdown voltages exceeding −17 V and maintain operational stability for over 3,000 h with negligible degradation. These findings underscore the effectiveness of a-SAMULs in enhancing the long-term reliability of perovskite photovoltaics.
This is a preview of subscription content, access via your institution
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$32.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Buy this article
USD 39.95
Prices may be subject to local taxes which are calculated during checkout
All data generated or analysed during this study are included in the Article and its Supplementary Information. Source data are provided with this paper.
Zhang, X. et al. Advances in inverted perovskite solar cells. Nat. Photonics 18, 1243–1253 (2024).
Article Google Scholar
Liu, C. et al. Bimolecularly passivated interface enables efficient and stable inverted perovskite solar cells. Science 382, 810–815 (2023).
Article Google Scholar
Li, M., Liu, M., Qi, F., Lin, F. R. & Jen, A. K. Self-assembled monolayers for interfacial engineering in solution-processed thin-film electronic devices: Design, fabrication, and applications. Chem. Rev. 124, 2138–2204 (2024).
Article Google Scholar
Khenkin, M. V. et al. Consensus statement for stability assessment and reporting for perovskite photovoltaics based on ISOS procedures. Nat. Energy 5, 35–49 (2020).
Article Google Scholar
Wu, S. et al. Redox mediator-stabilized wide-bandgap perovskites for monolithic perovskite-organic tandem solar cells. Nat. Energy 9, 411–421 (2024).
Article Google Scholar
Mariani, P. et al. Low-temperature strain-free encapsulation for perovskite solar cells and modules passing multifaceted accelerated ageing tests. Nat. Commun. 15, 4552 (2024).
Article Google Scholar
Ummadisingu, A. et al. The effect of illumination on the formation of metal halide perovskite films. Nature 545, 208–212 (2017).
Article Google Scholar
Wang, W.-T. et al. Water- and heat-activated dynamic passivation for perovskite photovoltaics. Nature 632, 294–300 (2024).
Article Google Scholar
Jiang, F. et al. Improved reverse bias stability in p–i–n perovskite solar cells with optimized hole transport materials and less reactive electrodes. Nat. Energy 9, 1275–1284 (2024).
Article Google Scholar
Diethelm, M. et al. Probing ionic conductivity and electric field screening in perovskite solar cells: a novel exploration through ion drift currents. Energy Environ. Sci. 18, 1385–1397 (2025).
Article Google Scholar
Wang, X. et al. Regulating phase homogeneity by self-assembled molecules for enhanced efficiency and stability of inverted perovskite solar cells. Nat. Photonics 18, 1269–1275 (2024).
Article Google Scholar
Yuan, Y. & Huang, J. Ion migration in organometal trihalide perovskite and its impact on photovoltaic efficiency and stability. Acc. Chem. Res. 49, 286–293 (2016).
Article Google Scholar
Chen, R. et al. Rear electrode materials for perovskite solar cells. Adv. Funct. Mater. 32, 2200651 (2022).
Article Google Scholar
Zhu, H. et al. Long-term operating stability in perovskite photovoltaics. Nat. Rev. Mater. 8, 569–586 (2023).
Article Google Scholar
Calado, P. et al. Evidence for ion migration in hybrid perovskite solar cells with minimal hysteresis. Nat. Commun. 7, 13831 (2016).
Article Google Scholar
Li, N. et al. Barrier reinforcement for enhanced perovskite solar cell stability under reverse bias. Nat. Energy 9, 1264–1274 (2024).
Article Google Scholar
Ni, Z. et al. Evolution of defects during the degradation of metal halide perovskite solar cells under reverse bias and illumination. Nat. Energy 7, 65–73 (2021).
Article Google Scholar
Xu, Z. et al. Halogen redox shuttle explains voltage-induced halide redistribution in mixed-halide perovskite devices. ACS Energy Lett. 8, 513–520 (2022).
Article Google Scholar
Kirmani, A. R. et al. Metal oxide barrier layers for terrestrial and space perovskite photovoltaics. Nat. Energy 8, 191–202 (2023).
Article Google Scholar
Huang, X. et al. Polyoxometalate reinforced perovskite phase for high-performance perovskite photovoltaics. Adv. Mater. 36, e2410564 (2024).
Article Google Scholar
Liu, J. et al. Efficient and stable perovskite-silicon tandem solar cells through contact displacement by MgFx. Science 377, 302–306 (2022).
Article Google Scholar
Ren, X. et al. Mobile iodides capture for highly photolysis- and reverse-bias-stable perovskite solar cells. Nat. Mater. 23, 810–817 (2024).
Article Google Scholar
Wu, W. et al. Stable and uniform self-assembled organic diradical molecules for perovskite photovoltaics. Science 389, 195–199 (2025).
Article Google Scholar
Liu, S. et al. Buried interface molecular hybrid for inverted perovskite solar cells. Nature 632, 536–542 (2024).
Article Google Scholar
Di Girolamo, D. et al. Silicon / perovskite tandem solar cells with reverse bias stability down to −40 V. Unveiling the role of electrical and optical design. Adv. Sci. 11, e2401175 (2024).
Article Google Scholar
Li, R., Gong, R., Lin, H., Green, M. A. & Lan, D. Reverse-bias challenges facing perovskite–silicon tandem solar cells under field conditions. Newton 1, 100001 (2025).
Article Google Scholar
Bertoluzzi, L. et al. Incorporating electrochemical halide oxidation into drift-diffusion models to explain performance losses in perovskite solar cells under prolonged reverse bias. Adv. Energy Mater. 11, 2002027 (2021).
Article Google Scholar
Thiesbrummel, J. et al. Ion-induced field screening as a dominant factor in perovskite solar cell operational stability. Nat. Energy 9, 664–676 (2024).
Article Google Scholar
Le Corre, V. M. et al. Quantification of efficiency losses due to mobile ions in perovskite solar cells via fast hysteresis measurements. Sol. RRL 6, 2100772 (2022).
Article Google Scholar
Li, D. et al. Co-adsorbed self-assembled monolayer enables high-performance perovskite and organic solar cells. Nat. Commun. 15, 7605 (2024).
Article Google Scholar
Xiong, W. et al. Controllable p- and n-type behaviours in emissive perovskite semiconductors. Nature 633, 344–350 (2024).
Article Google Scholar
He, R. et al. Improving interface quality for 1-cm2 all-perovskite tandem solar cells. Nature 618, 80–86 (2023).
Article Google Scholar
Tockhorn, P. et al. Nano-optical designs for high-efficiency monolithic perovskite–silicon tandem solar cells. Nat. Nanotechnol. 17, 1214–1221 (2022).
Article Google Scholar
Jiang, W. et al. π-expanded carbazoles as hole-selective self-assembled monolayers for high-performance perovskite solar cells. Angew. Chem. Int. Ed 134, e202213560 (2022).
Article Google Scholar
Jiang, W. et al. Spin-coated and vacuum-processed hole-extracting self-assembled multilayers with h-aggregation for high-performance inverted perovskite solar cells. Angew. Chem. Int. Ed 63, e202411730 (2024).
Article Google Scholar
Yu, S. et al. Homogenized NiOx nanoparticles for improved hole transport in inverted perovskite solar cells. Science 382, 1399–1404 (2023).
Article Google Scholar
Li, Z. et al. Stabilized hole-selective layer for high-performance inverted p–i–n perovskite solar cells. Science 382, 284–289 (2023).
Article Google Scholar
Ding, J., Rahman, O. U., Peng, W., Dou, H. & Yu, H. A novel hydroxyl epoxy phosphate monomer enhancing the anticorrosive performance of waterborne graphene/epoxy coatings. Appl. Surf. Sci. 427, 981–991 (2018).
Article Google Scholar
Luo, Y. et al. Understanding and measurement for the binding energy of hydrogen bonds of biomass-derived hydroxyl compounds. J. Phys. Chem. A 122, 843–848 (2018).
Article Google Scholar
Tuttle, M. R., Davis, S. T. & Zhang, S. Synergistic effect of hydrogen bonding and π–π stacking enables long cycle life in organic electrode materials. ACS Energy Lett. 6, 643–649 (2021).
Article Google Scholar
Liang, Y. et al. A matrix-confined molecular layer for perovskite photovoltaic modules. Nature 648, 91–96 (2025).
Stolterfoht, M. et al. The impact of energy alignment and interfacial recombination on the internal and external open-circuit voltage of perovskite solar cells. Energy Environ. Sci. 12, 2778–2788 (2019).
Article Google Scholar
Warby, J. et al. Mismatch of quasi-Fermi level splitting and Voc in perovskite solar cells. Adv. Energy Mater. 13, 202303135 (2023).
Article Google Scholar
Johnson, S. et al. How non-ohmic contact-layer diodes in perovskite pinholes affect abrupt low-voltage reverse-bias breakdown and destruction of solar cells. Joule 9, 102102 (2025).
Article Google Scholar
Diekmann, J. et al. Determination of mobile ion densities in halide perovskites via low-frequency capacitance and charge extraction techniques. J. Phys. Chem. Lett. 14, 4200–4210 (2023).
Article Google Scholar
Kühne, T. D. et al. CP2K: an electronic structure and molecular dynamics software package – quickstep: efficient and accurate electronic structure calculations. J. Chem. Phys. 152, 194103 (2020).
Article Google Scholar
van Setten, M. J. et al. The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table. Comput. Phys. Commun. 226, 39–54 (2018).
Article Google Scholar
Lu, T. A comprehensive electron wavefunction analysis toolbox for chemists, Multiwfn. J. Chem. Phys. 161, 082503 (2024).
Article Google Scholar
Lu, T. & Chen, F. Multiwfn: a multifunctional wavefunction analyzer. J. Comput. Chem. 33, 580–592 (2011).
Article Google Scholar
Humphrey, W., Dalke, A. & Schulten, K. VMD: Visual Molecular Dynamics. J. Mol. Graph. 14, 33–38 (1996).
Article Google Scholar
Delley, B. An all-electron numerical method for solving the local density functional for polyatomic molecules. J. Chem. Phys. 92, 508–517 (1990).
Article Google Scholar
Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).
Article Google Scholar
Goerigk, L. & Grimme, S. A thorough benchmark of density functional methods for general main group thermochemistry, kinetics, and noncovalent interactions. Phys. Chem. Chem. Phys. 13, 6670–6688 (2011).
Article Google Scholar
Johnson, E. R., Mackie, I. D. & DiLabio, G. A. Dispersion interactions in density-functional theory. J. Phys. Org. Chem. 22, 1127–1135 (2009).
Article Google Scholar
Kim, K.-H. et al. Phosphorescent dye-based supramolecules for high-efficiency organic light-emitting diodes. Nat. Commun. 5, 4769 (2014).
Article Google Scholar
Thompson, A. P. et al. LAMMPS – a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales. Comput. Phys. Commun. 271, 108171 (2022).
Article Google Scholar
Rappe, A. K., Casewit, C. J., Colwell, K. S., Goddard, W. A. & Skiff, W. M. UFF, a full periodic table force field for molecular mechanics and molecular dynamics simulations. J. Am. Chem. Soc. 114, 10024–10035 (2002).
Article Google Scholar
Swope, W. C., Andersen, H. C., Berens, P. H. & Wilson, K. R. A computer simulation method for the calculation of equilibrium constants for the formation of physical clusters of molecules: application to small water clusters. J. Chem. Phys. 76, 637–649 (1982).
Article Google Scholar
Hoover, W. G. Canonical dynamics: equilibrium phase-space distributions. Phys. Rev. A 31, 1695–1697 (1985).
Article Google Scholar
Hockney, R. W. & Eastwood, J. W. Computer Simulation Using Particles (CRC Press, 1966).
Download references
M.S. acknowledges funding support from The Chinese University of Hong Kong (CUHK) through the Vice-Chancellor Early Career Professorship Scheme, the Research Grants Council (RGC) under the NSCF/RGC Joint Research Scheme (N_CUHK414/24) and Young CRF scheme (C4069-25YF), and the Innovation and Technology Commission (ITC) via the ITF Seed Fund (ITS/239/23). A.K.Y.J. thanks the sponsorship of the Lee Shau-Kee Chair Professor (Materials Science), the MHKJFS grant (MHP/054/23), TCFS grant (GHP/121/22SZ), and MRP grant (MRP/040/21X) from the Innovation and Technology Commission of Hong Kong, and the GRF grants (11307621, 11316422, 11308625) and CRS grants (CRS_CityU104/23, CRS_HKUST203/23) from the Research Grants Council of Hong Kong. This work was partially supported by City University of Hong Kong (9610739) for the project ‘Fostering Innovation for Resilience and Sustainable Transformation,’ officially endorsed by the United Nations Educational, Scientific, and Cultural Organization under the International Decade of Sciences for Sustainable Development (2024–2033).
These authors contributed equally: Qifan Feng, Kai-Kai Liu, Deng Wang.
Electronic Engineering Department, The Chinese University of Hong Kong, Shatin, China
Qifan Feng, Zhaoyu Lou, Ziwei Liu, Nikhil Kalasariya & Martin Stolterfoht
Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, China
Kai-Kai Liu, Deng Wang, Songyang Yuan, Wenlin Jiang, Xiaofeng Huang & Alex K.-Y. Jen
Hong Kong Institute for Clean Energy, City University of Hong Kong, Kowloon, China
Kai-Kai Liu, Deng Wang, Wenlin Jiang, Xiaofeng Huang & Alex K.-Y. Jen
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, China
Zhenhuang Su
Department of Chemistry, City University of Hong Kong, Kowloon, China
Xin Wu, Zonglong Zhu & Alex K.-Y. Jen
School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, China
Shuo Zhang
Pen-Tung Sah Institute of Micro-Nano Science and Technology, Xiamen University, Xiamen, China
Binghui Wu
State Key Laboratory of Marine Environmental Health, City University of Hong Kong, Kowloon, China
Alex K.-Y. Jen
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
PubMed Google Scholar
Q.F., X.H., K.-K.L. and M.S. conceived the project. Q.F. and X.H. performed the experiments, analysed data and contributed to manuscript preparation. K.-K.L. designed and synthesized the molecules and conducted material characterizations. D.W. optimized device performance, S.Y. carried out the calculations and Z.S. conducted the GIWAXS measurements. Z.Lo., Z.Li., N.K., W.J., X.W., S.Z. and Z.Z. assisted with data interpretation and analysis. B.W. provided ToF-SIMS characterization. X.H., A.J. and M.S. finalized the manuscript with contributions from all authors.
Correspondence to Xiaofeng Huang, Alex K.-Y. Jen or Martin Stolterfoht.
M.S. is a co-founder of SolarSense Technologies Limited. The other authors declare no competing interests.
Nature Energy thanks Hong Li and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Peer reviewer reports are available.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Figs. 1–66, scheme 1 and Supplementary Tables 1–6.
Source data for Fig. 1.
Source data for Fig. 2.
Source data for Fig. 3.
Source data for Fig. 4.
Source data for Fig. 5.
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
Reprints and permissions
Feng, Q., Liu, KK., Wang, D. et al. Amorphous self-assembled multilayers for perovskite solar cells with improved reverse bias stability. Nat Energy (2026). https://doi.org/10.1038/s41560-026-02015-8
Download citation
Received:
Accepted:
Published:
Version of record:
DOI: https://doi.org/10.1038/s41560-026-02015-8
Anyone you share the following link with will be able to read this content:
Sorry, a shareable link is not currently available for this article.
Provided by the Springer Nature SharedIt content-sharing initiative
Advertisement
Nature Energy (Nat Energy)
ISSN 2058-7546 (online)
© 2026 Springer Nature Limited
Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.
