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Nature Materials (2026)
Regulation of electron- or hole-selective interfacial properties has traditionally relied on extrinsic chemical doping. Here we report a structurally driven strategy for modulating carrier-selective electronic characteristics through the organic-cation-induced reconfiguration of lead iodide octahedral connectivity. Two closely related imidazoline-based cations, which differ by only a single heteroatom, drive the formation of one-dimensional organic lead triiodide phases with distinct octahedral-sharing patterns. Single-crystal analysis combined with theoretical calculations reveals that the variation in connectivity reshapes orbital coupling, leading to pronounced changes in the work function and absolute band-edge positions that give rise to distinct carrier-selective interfacial behaviour without the introduction of extrinsic dopants. Leveraging this structural reconfiguration-induced electronic modulation, we realize complementary charge-selective contacts in perovskite solar cells, achieving a power conversion efficiency of 27.61% (certified steady-state 27.19%), together with excellent operational stability and scalability, including 22.26% efficiency in 655-cm2 modules.
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Kim, H.-S. et al. Lead iodide perovskite sensitized all-solid-state submicron thin film mesoscopic solar cell with efficiency exceeding 9%. Sci. Rep. 2, 591 (2012).
Article PubMed PubMed Central Google Scholar
Xiong, Z. et al. Homogenized chlorine distribution for >27% power conversion efficiency in perovskite solar cells. Science 390, 638–642 (2025).
Article CAS PubMed Google Scholar
Zhang, Y. et al. Dynamical transformation of two-dimensional perovskites with alternating cations in the interlayer space for high-performance photovoltaics. J. Am. Chem. Soc. 141, 2684–2694 (2019).
Article CAS PubMed Google Scholar
Liang, Z. et al. Homogenizing out-of-plane cation composition in perovskite solar cells. Nature 624, 557–563 (2023).
Article CAS PubMed PubMed Central Google Scholar
Cho, S.-H. et al. Solution-phase PbI2 coordination controls perovskite film formation and photovoltaic performance. ACS Energy Lett. 10, 3931–3940 (2025).
Article CAS Google Scholar
Canil, L. et al. Tuning halide perovskite energy levels. Energy Environ. Sci. 14, 1429–1438 (2021).
Article CAS Google Scholar
Peng, Y. et al. Enlarging moment and regulating orientation of buried interfacial dipole for efficient inverted perovskite solar cells. Nat. Commun. 16, 1252 (2025).
Article CAS PubMed PubMed Central Google Scholar
Zhang, C. et al. Work function tuning of a weak adhesion homojunction for stable perovskite solar cells. Joule 8, 1394–1411 (2024).
Article CAS Google Scholar
Zhang, J., Sun, Y. & Yu, H. Reducing energy loss via adjusting the anode work function and perovskite layer morphology for the efficient and stable hole transporting layer-free perovskite solar cells. Chem. Eng. J. 431, 133948 (2022).
Article CAS Google Scholar
Ren, B. et al. A universal p-type heterointerface for inverted perovskite solar cells. Angew. Chem. Int. Ed. 64, e202507950 (2025).
Article CAS Google Scholar
Liu, S. et al. Buried interface molecular hybrid for inverted perovskite solar cells. Nature 632, 536–542 (2024).
Article PubMed Google Scholar
Zhou, C. et al. Dual interfacial modification with 1D perovskite for self-assembled monolayer based inverted perovskite solar cells. Nano Energy 128, 109811 (2024).
Article CAS Google Scholar
Jeon, Y.-S. & Park, N.-G. Nickel oxide thin films formed from the pH-adjusted solutions for inverted perovskite solar cells. ACS Energy Lett. 10, 1266–1274 (2025).
Article CAS Google Scholar
Liu, G. et al. Mixed-phase low-dimensional perovskite-assisted interfacial lead directional management for stable perovskite solar cells with efficiency over 24%. ACS Energy Lett. 6, 4395–4404 (2021).
Article CAS Google Scholar
Xue, J. et al. Reconfiguring the band-edge states of photovoltaic perovskites by conjugated organic cations. Science 371, 636–640 (2021).
Article CAS PubMed Google Scholar
Li, M., Huang, P. & Zhong, H. Current understanding of band-edge properties of halide perovskites: Urbach tail, Rashba splitting, and exciton binding energy. J. Phys. Chem. Lett. 14, 1592–1603 (2023).
Article CAS PubMed Google Scholar
Daboczi, M. et al. Optimal interfacial band bending achieved by fine energy level tuning in mixed-halide perovskite solar cells. ACS Energy Lett. 6, 3970–3981 (2021).
Article CAS Google Scholar
Kutkan, S. et al. Impact of the organic cation on the band-edge emission of two-dimensional lead–bromide perovskites. Nanoscale 15, 12880–12888 (2023).
Article CAS PubMed Google Scholar
Li, X. et al. Constructing heterojunctions by surface sulfidation for efficient inverted perovskite solar cells. Science 375, 434–437 (2022).
Article CAS PubMed Google Scholar
Monika, Verma, A., Tiwari, M. K., Show, B. & Saha, S. Modulation of weak interactions in structural isomers: positional isomeric effects on crystal packing and physical properties and solid-state thin-film fabrication. ACS Omega 5, 448–459 (2019).
Article PubMed PubMed Central Google Scholar
Zeng, M. et al. Tailored supramolecular interface enables efficient and stable tin halide perovskite photovoltaics. ACS Energy Lett. 10, 1357–1365 (2025).
Article CAS Google Scholar
Dahlman, C. J., Kubicki, D. J. & Reddy, G. N. M. Interfaces in metal halide perovskites probed by solid-state NMR spectroscopy. J. Mater. Chem. A 9, 19206–19244 (2021).
Article CAS Google Scholar
Hui, W. et al. Stabilizing black-phase formamidinium perovskite formation at room temperature and high humidity. Science 371, 1359–1364 (2021).
Article CAS PubMed Google Scholar
Kang, D.-H., Park, Y.-J., Jeon, Y.-S. & Park, N.-G. Extended X-ray absorption fine structure (EXAFS) of FAPbI3 for understanding local structure–stability relation in perovskite solar cells. J. Energy Chem. 67, 549–554 (2022).
Article CAS Google Scholar
Zhang, B. et al. Inhibiting ion migration and stabilizing crystal-phase in halide perovskite via directly incorporated fluoride anion. Angew. Chem. Int. Ed. 137, e202413550 (2025).
Article Google Scholar
Wen, Y. et al. Amorphous (lysine)2PbI2 layer enhanced perovskite photovoltaics. Nat. Commun. 15, 7085 (2024).
Article CAS PubMed PubMed Central Google Scholar
Sanson, A. EXAFS spectroscopy: a powerful tool for the study of local vibrational dynamics. Microstructures 1, 2021004 (2021).
Google Scholar
Ibaceta-Jaña, J. et al. Vibrational dynamics in lead halide hybrid perovskites investigated by Raman spectroscopy. Phys. Chem. Chem. Phys. 22, 5604–5614 (2020).
Article PubMed Google Scholar
Zheng, J. et al. Incorporation of CoO nanoparticles in 3D marigold flower-like hierarchical architecture MnCo2O4 for highly boosting solar light photo-oxidation and reduction ability. App. Catal. B 237, 1–8 (2018).
Article CAS Google Scholar
Yang, Y. et al. Inverted perovskite solar cells with over 2,000 h operational stability at 85 °C using fixed charge passivation. Nat. Energy 9, 37–46 (2024).
Article CAS Google Scholar
Ji, R. et al. Spontaneous formation of 1D/3D perovskite heterojunctions for efficient inverted perovskite solar cells. Adv. Energy Mater. 14, 2304126 (2024).
Article CAS Google Scholar
Wei, N. et al. Post-treatment-free dual-interface passivation via facile 1D/3D perovskite heterojunction construction. JACS Au 3, 3324–3332 (2023).
Article CAS PubMed PubMed Central Google Scholar
Chen, R. et al. Conformal imidazolium 1D perovskite capping layer stabilized 3D perovskite films for efficient solar modules. Adv. Sci. 9, 2204017 (2022).
Article CAS Google Scholar
Jiao, H. et al. Perovskite grain wrapping by converting interfaces and grain boundaries into robust and water-insoluble low-dimensional perovskites. Sci. Adv. 8, eabq4524 (2022).
Article CAS PubMed PubMed Central Google Scholar
Xiong, W. et al. Controllable p-and n-type behaviours in emissive perovskite semiconductors. Nature 633, 344–350 (2024).
Article CAS PubMed Google Scholar
Xiong, S. et al. Direct observation on p- to n-type transformation of perovskite surface region during defect passivation driving high photovoltaic efficiency. Joule 5, 467–480 (2021).
Article CAS Google Scholar
Zheng, Y. et al. Towards 26% efficiency in inverted perovskite solar cells via interfacial flipped band bending and suppressed deep-level traps. Energy Environ. Sci. 17, 1153–1162 (2024).
Article CAS Google Scholar
Al-Ashouri, A. et al. Monolithic perovskite/silicon tandem solar cell with >29% efficiency by enhanced hole extraction. Science 370, 1300–1309 (2020).
Article CAS PubMed Google Scholar
Cacovich, S. et al. Imaging and quantifying non-radiative losses at 23% efficient inverted perovskite solar cells interfaces. Nat. Commun. 13, 2868 (2022).
Article CAS PubMed PubMed Central Google Scholar
Xu, H. et al. Constructing robust heterointerfaces for carrier viaduct via interfacial molecular bridges enables efficient and stable inverted perovskite solar cells. Energy Environ. Sci. 16, 5792–5804 (2023).
Article CAS Google Scholar
Ye, F. et al. Overcoming C60-induced interfacial recombination in inverted perovskite solar cells by electron-transporting carborane. Nat. Commun. 13, 7454 (2022).
Article CAS PubMed PubMed Central Google Scholar
Warby, J. et al. Mismatch of quasi-Fermi level splitting and Voc in perovskite solar cells. Adv. Energy Mater. 13, 2303135 (2023).
Article CAS Google Scholar
Caprioglio, P. et al. Open-circuit and short-circuit loss management in wide-gap perovskite p-i-n solar cells. Nat. Commun. 14, 932 (2023).
Article CAS PubMed PubMed Central Google Scholar
Duan, C. et al. Scalable fabrication of wide-bandgap perovskites using green solvents for tandem solar cells. Nat. Energy 10, 318–328 (2025).
Article CAS Google Scholar
Sarritzu, V. et al. Optical determination of Shockley–Read–Hall and interface recombination currents in hybrid perovskites. Sci. Rep. 7, 44629 (2017).
Article CAS PubMed PubMed Central Google Scholar
Kresse, G. & Hafner, J. Ab initio molecular dynamics for open-shell transition metals. Phys. Rev. B 48, 13115–13118 (1993).
Article CAS Google Scholar
Kresse, G. & Nafner, J. Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium. Phys. Rev. B 49, 14251–14269 (1994).
Article CAS Google Scholar
Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).
Article CAS PubMed Google Scholar
Monkhorst, H. J. & Pack, J. D. Special points for Brillouin-zone integrations. Phys. Rev. B 13, 5188–5192 (1976).
Article Google Scholar
Grimme, S., Antony, J., Ehrlich, S. & Krieg, H. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H–Pu. J. Chem. Phys. 132, 154104 (2010).
Article PubMed Google Scholar
Dronskowski, R. & Blöchl, P. E. Crystal orbital Hamilton populations (COHP): energy-resolved visualization of chemical bonding in solids based on density-functional calculations. J. Phys. Chem. 97, 8617–8624 (1993).
Article CAS Google Scholar
Deringer, V. L., Tchougréeff, A. L. & Dronskowski, R. Crystal orbital Hamilton population (COHP) analysis as projected from plane-wave basis sets. J. Phys. Chem. 115, 5461–5466 (2011).
Article CAS Google Scholar
Maintz, S., Deringer, V. L., Tchougréeff, A. L. & Dronskowski, R. LOBSTER: a tool to extract chemical bonding from plane-wave based DFT. J. Comput. Chem. 37, 1030–1035 (2016).
Article CAS PubMed PubMed Central Google Scholar
Hoover, W. G. Canonical dynamics: equilibrium phase-space distributions. Phys. Rev. A 31, 1695–1697 (1985).
Article CAS Google Scholar
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This work was supported by National Research Foundation of Korea (NRF) grants funded by the Korean government (MSIT and MOE) under contracts RS-2026-25501632 (NRL 2.0), NRF-2021R1A3B1076723 (Research Leader Program), RS-2025-02316700 (Carbon-free Energy Core Technology Program), RS-2023-00259096 (GRDC Cooperative Hub) and the Ministry of Trade, Industry and Energy (MOTIE) of Korea (P0022336). We thank the Shanghai Synchrotron Radiation Facility for use of the BL17B1 and BL13SSW beamlines (cstr.cn/31124.02.SSRF.BL13SSW) and for support with the XAFS experiments.
These authors contributed equally: Yalan Zhang, Zheng Liang.
School of Chemical Engineering and Center for Antibonding Regulated Crystals, Sungkyunkwan University, Suwon, Republic of Korea
Yalan Zhang, Zheng Liang, Seong Chan Cho, Seong-Ho Cho, Guiming Fu, Sang-Uk Lee, Sanwan Liu & Nam-Gyu Park
School of Chemical Engineering, Sungkyunkwan University, Suwon, Republic of Korea
Seong Chan Cho, Jae Hun Seol & Sang Uck Lee
Key Laboratory of Applied Surface and Colloid Chemistry, National Ministry of Education, Shaanxi Key Laboratory for Advanced Energy Devices, Shaanxi Engineering Lab for Advanced Energy Technology and School of Materials Science and Engineering, Shaanxi Normal University, Xi’an, People’s Republic of China
Xin Chen & Kui Zhao
University of Science and Technology of China, Hefei, People’s Republic of China
Boyuan Liu, Hui Zhang & Xu Pan
School of Microelectronics, Hefei University of Technology, Hefei, People’s Republic of China
Xu Pan
SKKU National Lab for Intelligent Energy Solution Technology (SIEST), Sungkyunkwan University, Suwon, Republic of Korea
Nam-Gyu Park
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Y.Z., Z.L. and N.-G.P. conceived the study. N.-G.P. supervised the project. Y.Z. and Z.L. fabricated the perovskite devices, performed the photovoltaic characterizations and analysed the experimental data. Y.Z. and Z.L. wrote the paper. N.-G.P. revised and edited the paper. G.F. performed the KPFM measurements. B.L. and H.Z. assisted with the EXAFS analysis. X.C. conducted and analysed the GIWAXS measurements under the supervision of K.Z. The XRD measurements were performed by S.-U.L. The DFT calculations were carried out by S.C.C. and J.H.S. under the supervision of S.U.L. Analysis of the NMR data was assisted by S.-H.C. and S.L. All authors discussed the results and contributed to the paper.
Correspondence to Sang Uck Lee, Xu Pan or Nam-Gyu Park.
The authors declare no competing interests.
Nature Materials thanks Milos Dubajic 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. 1–39; Tables 1–11, Notes 1–4 and refs. 1 and 2.
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Zhang, Y., Liang, Z., Cho, S.C. et al. Octahedral connectivity reconfigures interfacial carrier-selective properties for efficient perovskite solar cells. Nat. Mater. (2026). https://doi.org/10.1038/s41563-026-02722-3
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