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Lateral epitaxial growth of two-dimensional organic heterostructures

Nature Chemistry volume 16, pages 201–209 (2024)Cite this article

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Abstract

Two-dimensional organic lateral heterostructures (2D OLHs) are attractive for the fabrication of functional materials. However, it is difficult to control the nucleation, growth and orientation of two distinct components. Here we report the combination of two methods—liquid-phase growth and vapour-phase growth—to synthesize 2D OLHs from perylene and a perylenecarboxaldehyde derivative, with a lateral size of ~20 μm and a tunable thickness ranging from 20 to 400 nm. The screw dislocation growth behaviour of the 2D crystals shows the spiral arrangement of atoms within the crystal lattice, which avoids volume expansion and contraction of OLH, thereby minimizing lateral connection defects. Selective control of the nucleation and sequential growth of 2D crystals leads to structural inversion of the 2D OLHs by the vapour-phase growth method. The resulting OLHs show good light-transport capabilities and tunable spatial exciton conversion, useful for photonic applications. This synthetic strategy can be extended to other families of organic polycyclic aromatic hydrocarbons, as demonstrated with other pyrene and perylene derivatives.

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Fig. 1: Two-step strategy for the synthesis of 2D OLHs with structural inversion.
Fig. 2: Characterizations of Pe−PeO lateral heterostructures.
Fig. 3: Characterizations of PeO−Pe lateral heterostructures.
Fig. 4: Optical applications of two lateral heterostructures.
Fig. 5: General synthesis of OLHs.

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Data availability

Crystallographic data for the structures reported in this Article have been deposited at the Cambridge Crystallographic Data Centre, under deposition numbers CCDC 1546182 (Pe) and 2203762 (PeO). Copies of the data can be obtained free of charge at https://www.ccdc.cam.ac.uk/structures/. All data are available in the main Article and Supplementary Information. Source data are provided with this paper.

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Acknowledgements

X.-D.W. acknowledges financial support from the National Natural Science Foundation of China (nos. 21971185 and 52173177), the Natural Science Foundation of Jiangsu Province (no. BK20221362) and the Science and Technology Support Program of Jiangsu Province (no. TJ-2022-002). This work was also supported by the Suzhou Key Laboratory of Functional Nano & Soft Materials, the Collaborative Innovation Center of Suzhou Nano Science & Technology, the 111 Project, the Joint International Research Laboratory of Carbon-Based Functional Materials and Devices and Soochow University Tang Scholar scheme.

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Authors and Affiliations

  1. Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices, Soochow University, Suzhou, Jiangsu, PR China

    Qiang Lv, Xue-Dong Wang, Yue Yu, Chao-Fei Xu, Yan-Jun Yu, Xing-Yu Xia & Liang-Sheng Liao

  2. National Engineering Laboratory for Modern Silk, College of Textile and Clothing Engineering, Research Center of Cooperative Innovation for Functional Organic/Polymer Material Micro/Nanofabrication, Soochow University, Suzhou, Jiangsu, PR China

    Qiang Lv & Min Zheng

  3. Macao Institute of Materials Science and Engineering, Macau University of Science and Technology, Taipa, Macau SAR, PR China

    Liang-Sheng Liao

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Contributions

X.-D.W., M.Z. and L.-S.L. conceived the project. Q.L. synthesized the 2D organic lateral heterostructures and investigated their growth mechanism. Q.L. conducted the SEM, FM and Raman measurements and data analysis. Y.Y. performed the optical characterizations. C.-F.X. and X.-Y.X. carried out the AFM and solubility measurements. Y.-J.Y. conducted the TEM measurements. All authors discussed the results. Q.L. wrote the paper with input from all of the authors. The project was supervised by X.-D.W., M.Z. and L.-S.L.

Corresponding authors

Correspondence to Xue-Dong Wang, Min Zheng or Liang-Sheng Liao.

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Nature Chemistry thanks Wai-Yeung Wong and the other, anonymous, reviewer for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–41, Tables 1–5, Notes 1–3 and References.

Supplementary Data 1

Crystal CIF for Pe single crystals.

Supplementary Data 2

Crystal CIF for PeO single crystals.

Supplementary Data 3

Source Data for Supplementary Figs. 5, 13, 19, 21, 24, 29, 30, 31, 32, 33 and 35.

Source data

Source Data Fig. 1

Unprocessed fluorescence microscopy images.

Source Data Fig. 2

Statistical source data.

Source Data Fig. 3

Statistical source data.

Source Data Fig. 4

Statistical source data.

Source Data Fig. 5

Statistical source data.

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Lv, Q., Wang, XD., Yu, Y. et al. Lateral epitaxial growth of two-dimensional organic heterostructures. Nat. Chem. 16, 201–209 (2024). https://doi.org/10.1038/s41557-023-01364-1

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