Abstract
Moiré superlattices have emerged as a new platform for studying strongly correlated quantum phenomena, but these systems have been largely limited to van der Waals layer two-dimensional materials. Here we introduce moiré superlattices leveraging ultrathin, ligand-free halide perovskites, facilitated by ionic interactions. Square moiré superlattices with varying periodic lengths are clearly visualized through high-resolution transmission electron microscopy. Twist-angle-dependent transient photoluminescence microscopy and electrical characterizations indicate the emergence of localized bright excitons and trapped charge carriers near a twist angle of ~10°. The localized excitons are accompanied by enhanced exciton emission, attributed to an increased oscillator strength by a theoretically predicted flat band. This research showcases the promise of two-dimensional perovskites as unique room-temperature moiré materials.
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All data that support the findings of this study are available from the corresponding authors on reasonable request. Source data are provided with this paper.
References
Cao, Y. et al. Unconventional superconductivity in magic-angle graphene superlattices. Nature 556, 43–50 (2018).
Ma, L. et al. Strongly correlated excitonic insulator in atomic double layers. Nature 598, 585–589 (2021).
Halbertal, D. et al. Multilayered atomic relaxation in van der Waals heterostructures. Phys. Rev. X 13, 011026 (2023).
Naik, M. H. et al. Intralayer charge-transfer moiré excitons in van der Waals superlattices. Nature 609, 52–57 (2022).
Song, Z. et al. Deep quantum-dot arrays in moiré superlattices of non-van der Waals materials. J. Am. Chem. Soc. 144, 14657–14667 (2022).
Kennes, D. M. et al. Moiré heterostructures as a condensed-matter quantum simulator. Nat. Phys. 17, 155–163 (2021).
Zhang, L., Zhang, X. & Lu, G. Predictions of moiré excitons in twisted two-dimensional organic–inorganic halide perovskites. Chem. Sci. 12, 6073–6080 (2021).
Weeks, C. & Franz, M. Topological insulators on the Lieb and perovskite lattices. Phys. Rev. B 82, 085310 (2010).
Dou, L. et al. Atomically thin two-dimensional organic–inorganic hybrid perovskites. Science 349, 1518–1521 (2015).
Leng, K. et al. Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation. Nat. Mater. 17, 908–914 (2018).
Stoumpos, C. C. et al. Ruddlesden–Popper hybrid lead iodide perovskite 2D homologous semiconductors. Chem. Mater. 28, 2852–2867 (2016).
Blancon, J. C. et al. Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites. Science 355, 1288–1292 (2017).
Wang, Y. et al. Chemical vapor deposition growth of single-crystalline cesium lead halide microplatelets and heterostructures for optoelectronic applications. Nano Res. 10, 1223–1233 (2017).
Liu, Y., Yang, Z. & Liu, S. Recent progress in single-crystalline perovskite research including crystal preparation, property evaluation, and applications. Adv. Sci. 5, 1700471 (2018).
Gao, Y. & Dou, L. Organic semiconductor-incorporated two-dimensional halide perovskites. Natl Sci. Rev. https://doi.org/10.1093/nsr/nwab111 (2021).
Gao, Y. et al. Molecular engineering of organic–inorganic hybrid perovskites quantum wells. Nat. Chem. 11, 1151–1157 (2019).
Akriti et al. Layer-by-layer anionic diffusion in two-dimensional halide perovskite vertical heterostructures. Nat. Nanotechnol. 16, 584–591 (2021).
Yang, A. et al. Giant enhancement of photoluminescence emission in WS2-two-dimensional perovskite heterostructures. Nano Lett. 19, 4852–4860 (2019).
Shi, E. et al. Two-dimensional halide perovskite lateral epitaxial heterostructures. Nature 580, 614–620 (2020).
Pan, D. et al. Deterministic fabrication of arbitrary vertical heterostructures of two-dimensional Ruddlesden–Popper halide perovskites. Nat. Nanotechnol. 16, 159–165 (2021).
Tabuchi, Y. et al. Preparation and characterization of natural lower dimensional layered perovskite-type compounds. J. Phys. Chem. Solids 61, 837–845 (2000).
Niu, W., Eiden, A., Prakash, G. V. & Baumberg, J. J. Exfoliation of self-assembled 2D organic-inorganic perovskite semiconductors. Appl. Phys. Lett. 104, 171111 (2014).
Li, P. et al. Two-dimensional CH3NH3PbI3 perovskite nanosheets for ultrafast pulsed fiber lasers. ACS Appl. Mater. Interfaces 9, 12759–12765 (2017).
Liu, J. et al. Two-dimensional CH3NH3PbI3 perovskite: synthesis and optoelectronic application. ACS Nano 10, 3536–3542 (2016).
Wang, Z. et al. Degradation of two-dimensional CH3NH3PbI3 perovskite and CH3NH3PbI3/graphene heterostructure. ACS Appl. Mater. Interfaces 10, 24258–24265 (2018).
Wang, Y. et al. Two-dimensional van der Waals epitaxy kinetics in a three-dimensional perovskite halide. Cryst. Growth Des. 15, 4741–4749 (2015).
Sun, Y. et al. Engineering the phases and heterostructures of ultrathin hybrid perovskite nanosheets. Adv. Mater. 32, 2002392 (2020).
Adjokatse, S. et al. Scalable fabrication of high-quality crystalline and stable FAPbI3 thin films by combining doctor-blade coating and the cation exchange reaction. Nanoscale 11, 5989–5997 (2019).
Reus, M. A. et al. Time-resolved orientation and phase analysis of lead halide perovskite film annealing probed by in situ GIWAXS. Adv. Opt. Mater. 10, 2102722 (2022).
Blancon, J. C. et al. Scaling law for excitons in 2D perovskite quantum wells. Nat. Commun. 9, 2254 (2018).
Yang, Y. et al. Comparison of recombination dynamics in CH3NH3PbBr3 and CH3NH3PbI3 perovskite films: influence of exciton binding energy. J. Phys. Chem. Lett. 6, 4688–4692 (2015).
Dyksik, M. et al. Tuning the excitonic properties of the 2D (PEA)2(MA)n–1PbnI3n+1 perovskite family via quantum confinement. J. Phys. Chem. Lett. 12, 1638–1643 (2021).
Zhu, H. et al. Lead halide perovskite nanowire lasers with low lasing thresholds and high quality factors. Nat. Mater. 14, 636–642 (2015).
Akselrod, G. M. et al. Subdiffusive exciton transport in quantum dot solids. Nano Lett. 14, 3556–3562 (2014).
Li, W. et al. Direct characterization of carrier diffusion in halide-perovskite thin films using transient photoluminescence imaging. ACS Photonics 6, 2375–2380 (2019).
Saidaminov, M. I. et al. Multi-cation perovskites prevent carrier reflection from grain surfaces. Nat. Mater. 19, 412–418 (2020).
Deng, S. et al. Long-range exciton transport and slow annihilation in two-dimensional hybrid perovskites. Nat. Commun. 11, 664 (2020).
Brem, S. et al. Hybridized intervalley moiré excitons and flat bands in twisted WSe2 bilayers. Nanoscale 12, 11088–11094 (2020).
Choi, J. et al. Moiré potential impedes interlayer exciton diffusion in van der Waals heterostructures. Sci. Adv. 6, eaba8866 (2020).
Zhang, L. et al. Van der Waals heterostructure polaritons with moiré-induced nonlinearity. Nature 591, 61–65 (2021).
Basov, D. N. et al. Polariton panorama. Nanophotonics 10, 549–577 (2021).
Su, R. et al. Observation of exciton polariton condensation in a perovskite lattice at room temperature. Nat. Phys. 16, 301–306 (2020).
Yu, Y. et al. Tunable angle-dependent electrochemistry at twisted bilayer graphene with moiré flat bands. Nat. Chem. 14, 267–273 (2022).
Acknowledgements
This work is primarily supported by the US Department of Energy, Office of Basic Energy Sciences, under award no. DE-SC0022082 (S.Z., L.J., L.D. and L.H.). The views expressed herein do not necessarily represent the views of the US Department of Energy or the United States government. L.D. acknowledges support from the National Science Foundation under award no. 2143568-DMR. The TEM work is supported by the Center for High-Resolution Electron Microscopy (CħEM) at ShanghaiTech University and the Shanghai Key Laboratory of High-Resolution Electron Microscopy (Y.L. and Y.Y.). E.M. acknowledges support from the German Research Foundation (DFG) via the CRC 1083 (project B9) as well as the regular project 504846924. G.L. acknowledges support from the US NSF PREM program (DMR-1828019) and the US Army Research Office (W911NF-23-10205). A.M.-K. acknowledges support from the School of Materials Engineering at Purdue University.
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L.D., L.H. and S.Z. designed the experiments. S.Z. synthesized and characterized all the 2D perovskite samples. L.J., D.B., S.K., Q.Z. and D.S. performed the optical properties characterizations and data analysis. Y.L., B.Y. and Y.Y. performed the TEM characterization and data analysis. J.Y.P. and S.Z. performed the confocal PL imaging on all the perovskite samples. L.Z., G.L., J.Y., J.J.P.T., E.M. and A.M.-K. performed the DFT and microscopic simulations as well as data analysis. Y.L. and S.Z. performed the device fabrication and characterization. B.P.F., A., Z.W., K.M. and H.P. participated in the materials characterization and data analysis. S.Z., L.D. and L.H. wrote the paper; all authors read and revised the paper.
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Nature Materials thanks Michael Saliba and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
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Supplementary Text, Supplementary Figures 1–65, Supplementary Tables 1–10 and References and Notes.
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Source Data Fig. 1
PL source data, XRD signal data and AFM height profile.
Source Data Fig. 3
Time-resolved PL imaging of exciton diffusion data, exciton density distribution data, exciton diffusion coefficient data and TRPL decay data.
Source Data Fig. 4
Steady-state PL emission spectrum in twisted samples, summary of angle-dependent PL emission and temperature-dependent PL intensities.
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Zhang, S., Jin, L., Lu, Y. et al. Moiré superlattices in twisted two-dimensional halide perovskites. Nat. Mater. 23, 1222–1229 (2024). https://doi.org/10.1038/s41563-024-01921-0
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DOI: https://doi.org/10.1038/s41563-024-01921-0
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