Abstract
Achieving the preferred orientation of specific facets is crucial for regulating the anisotropic physical properties of crystal materials and optimizing the performance of semiconductor optoelectronic devices. However, the intrinsic challenges lie in precisely controlling the growth kinetics of crystal facets and suppressing defects during the spontaneous crystallization processes. Herein, we report the microdroplet interface synthesis of Cs2AgBiBr6 single crystals with controlled orientations. By selectively reducing the nucleation barrier of (111) facets via modulation of the solid-liquid interface energy, the random (100)/(110)/(111) orientations are transformed into a selective (111)-preferred orientation. Further, thermal annealing is demonstrated to effectively improve crystal quality by releasing lattice strain and promoting octahedral reordering. Both theoretical calculations and experiments validate the advantages of (111)-oriented facets with higher ionic migrate energy and lower defect density than (100) and (110) facets, which result in better endurance to moisture and light irradiation. Besides, photodetectors based on the (111) facets exhibit superior performance to (100) and (110) facets. This work highlights the crucial role of interface energy in directing crystallographic orientation, providing theoretical basis and design strategies for the precise manipulation of crystal facets.
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References
Zhao, L. et al. High-yield growth of FACsPbBr3 single crystals with low defect density from mixed solvents for gamma-ray spectroscopy. Nat. Photon. 17, 315–323 (2023).
Chen, G. Y. et al. Nucleation-mediated growth of chiral 3D organic-inorganic perovskite single crystals. Nat. Chem. 15, 1581–1590 (2023).
Cao, F. et al. Lead-free single crystal metal halide perovskite detectors. Mater. Sci. Eng. R. 164, 100991 (2025).
Zhang, Y. X. et al. Nucleation-controlled growth of superior lead-free perovskite Cs3Bi2I9 single-crystals for high-performance X-ray detection. Nat. Commun. 11, 2304 (2020).
Connor, B. A., Leppert, L., Smith, M. D., Neaton, J. B. & Karunadasa, H. I. Layered halide double perovskites: dimensional reduction of Cs2AgBiBr6. J. Am. Chem. Soc. 140, 5235–5240 (2018).
Yu, W. J. et al. Breaking the bottleneck of lead-free perovskite solar cells through dimensionality modulation. Chem. Soc. Rev. 53, 1769–1788 (2024).
Zhang, X. et al. Self-assembly of 2D hybrid double perovskites on 3D Cs2AgBiBr6 crystals towards ultrasensitive detection of weak polarized light. Angew. Chem. Int. Ed. 61, e202205939 (2022).
Pan, W. C. et al. Cs2AgBiBr6 single-crystal X-ray detectors with a low detection limit. Nat. Photon. 11, 726–732 (2017).
Deng, M., Li, Z. Q., Liu, S. Y., Fang, X. S. & Wu, L. M. Wafer-scale integration of two-dimensional perovskite oxides towards motion recognition. Nat. Commun. 15, 8789 (2024).
Zhang, X., Li, Z., Hong, E., Yan, T. & Fang, X. Effective dual cation release in quasi-2D perovskites for ultrafast UV light-powered imaging. Adv. Mater. 37, 2412014 (2024).
Hu, Y. et al. High-purity photoactive α-phase for flexible perovskite photodetectors with modified electron transport layer. Adv. Funct. Mater. 35, 2412015 (2025).
Hong, E., Li, Z., Zhang, X., Fan, X. & Fang, X. Deterministic fabrication and quantum-well modulation of phase-pure 2D perovskite heterostructures for encrypted light communication. Adv. Mater. 36, 2400365 (2024).
Wei, Y. et al. Recent progress of bismuth effect on all-inorganic lead-free metal halide derivatives: crystals structure, luminescence properties, and applications. Adv. Funct. Mater. 33, 2205829 (2023).
Feng, J. G., Qiu, Y. C., Jiang, L. & Wu, Y. C. Long-range-ordered assembly of micro-/nanostructures at superwetting interfaces. Adv. Mater. 34, 2106857 (2022).
Ricciardulli, A. G., Yang, S., Smet, J. H. & Saliba, M. Emerging perovskite monolayers. Nat. Mater. 20, 1325–1336 (2021).
Pan, L. F. et al. High carrier mobility along the [111] orientation in Cu2O photoelectrodes. Nature 628, 765–770 (2024).
Dong, S. H. et al. All-inorganic perovskite single-crystal photoelectric anisotropy. Adv. Mater. 34, 2204342 (2022).
Wang, Y. et al. Facet engineering and pore design boost dynamic Fe exchange in oxygen evolution catalysis to break the activity-stability trade-off. J. Am. Chem. Soc. 145, 20261–20272 (2023).
Liu, Z. et al. All-perovskite tandem solar cells achieving >29% efficiency with improved (100) orientation in wide-bandgap perovskites. Nat. Mater. 24, 252–259 (2025).
Hsiao, Y. C. et al. A library of seed@high-entropy-alloy core-shell nanocrystals with controlled facets for catalysis. Adv. Mater. 37, 2411464 (2025).
Xia, P. et al. Improved facet and edge passivation in near-infrared III-V colloidal quantum dot photodetectors. Adv. Mater. 37, 2419020 (2025).
Yao, Y. X. et al. Oriented wide-bandgap perovskites for monolithic silicon-based tandems with over 1000 hours operational stability. Nat. Commun. 16, 40 (2025).
Ma, C. Q. et al. Unveiling facet-dependent degradation and facet engineering for stable perovskite solar cells. Science 379, 173–178 (2023).
Xia, M. et al. Kinetic Wulff-shaped heteroepitaxy of phase-pure 2D perovskite heterostructures with deterministic slab thickness. Nat. Synth. 4, 380–390 (2025).
Read, C. G., Steinmiller, E. M. P. & Choi, K. S. Atomic pane-selective deposition of gold nanoparticles on metal oxide crystals exploiting preferential adsorption of additives. J. Am. Chem. Soc. 131, 12040–12041 (2009).
Shi, Z. et al. Self-regulated facet stability during solution growth of perovskite crystals. Nat. Synth. 4, 1088–1094 (2025).
Wang, J. W. et al. Facet-engineered growth of non-layered 2D manganese chalcogenides. Adv. Powder Mater. 3, 100164 (2024).
Chen, C. S. et al. Fluid chemistry of metal halide perovskites. Angew. Chem. Int. Ed. 64, e202503593 (2025).
Hong, E., Li, Z., Yan, T. & Fang, X. Surface-tension-dominant crystallization of 2D perovskite single crystals for vertically oriented hetero-/homo-structure photodetectors. Nano Lett. 22, 8662–8669 (2022).
Zhang, Y. et al. Crystal facet engineering on SrTiO3 enhances photocatalytic overall water splitting. J. Am. Chem. Soc. 146, 6618–6627 (2024).
Prydatko, A. V., Belyaeva, L. A., Jiang, L., Lima, L. M. C. & Schneider, G. F. Contact angle measurement of free-standing square-millimeter single-layer graphene. Nat. Commun. 9, 4185 (2018).
Qu, S. J. et al. Revealing and inhibiting the facet-related ion migration for efficient and stable perovskite solar cells. Angew. Chem. Int. Ed. 64, e202415949 (2024).
Akriti et al. Layer-by-layer anionic diffusion in two-dimensional halide perovskite vertical heterostructures. Nat. Nanotechnol. 16, 584–591 (2021).
Jiang, J. et al. Synergistic strain engineering of perovskite single crystals for highly stable and sensitive X-ray detectors with low-bias imaging and monitoring. Nat. Photon. 16, 575–581 (2022).
Yang, X. Y. et al. In-line tempering eliminates the domain boundary in perovskite single crystals for high-energy resolution ionizing radiation detectors. Sci. Adv. 10, eadq6866 (2024).
Shen, Y. X. et al. Strain regulation retards natural operation decay of perovskite solar cells. Nature 635, 882–889 (2024).
Nagabhushana, G. P., Shivaramaiah, R. & Navrotsky, A. Direct calorimetric verification of thermodynamic instability of lead halide hybrid perovskites. Proc. Natl. Acad. Sci. USA. 113, 7717–7721 (2016).
Wang, F., Zhang, T., Xie, R. Z., Wang, Z. & Hu, W. D. How to characterize figures of merit of two-dimensional photodetectors. Nat. Commun. 14, 2224 (2023).
Wang, Z. Y., Wang, M. C., Heine, T. & Feng, X. L. Electronic and quantum properties of organic two-dimensional crystals. Nat. Rev. Mater. 10, 147–166 (2025).
Acknowledgements
This work was supported by the National Natural Science Foundation of China (Nos. 52425308 (X.F.), 524B2017 (E.H.), 62374035 (X.F.) and 92263106 (X.F.)).
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Z.L., L.W. and X.F. conceived the idea. Z.L. and E.H. designed the experiments. E.H. carried out the material synthesis and related characteristics. M.D. provided helpful suggestions about crystal growth and TRPL measurements. E.H., Z.L. and X.F. wrote and revised the manuscript. All authors reviewed and approved the paper.
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Hong, E., Li, Z., Deng, M. et al. Solid-liquid interface synthesis of selective (111)-oriented Cs2AgBiBr6 perovskite crystals. Nat Commun (2026). https://doi.org/10.1038/s41467-026-69926-8
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DOI: https://doi.org/10.1038/s41467-026-69926-8


