Abstract
Twist angle between two-dimensional layers is a critical parameter that determines their interfacial properties, such as moiré excitons and interfacial ferro-electricity. To achieve better control over these properties for fundamental studies and various applications, considerable efforts have been made to manipulate twist angle. However, due to mechanical limitations and the inevitable formation of incommensurate regions, there remains a challenge in attaining perfect alignment of crystalline orientation. Here we report a thermally induced atomic reconstruction of randomly stacked transition metal dichalcogenide multilayers into fully commensurate heterostructures with zero twist angle by encapsulation annealing, regardless of twist angles of as-stacked samples and lattice mismatches. We also demonstrate the selective formation of R- and H-type fully commensurate phases with a seamless lateral junction using chemical vapour-deposited transition metal dichalcogenides. The resulting fully commensurate phases exhibit strong photoluminescence enhancement of the interlayer excitons, even at room temperature, due to their commensurate structure with aligned momentum coordinates. Our work not only demonstrates a way to fabricate zero-twisted, two-dimensional bilayers with R- and H-type configurations, but also provides a platform for studying their unexplored properties.
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Acknowledgements
This work was supported by National Research Foundation of Korea Grants funded by the Korean Government (nos. 2021R1A2C3014316, 2021M3F3A2A01037858 and 2017R1A5A1014862 (SRC programme: vdWMRC centre)) and the Creative-Pioneering Researchers Programme through Seoul National University. S.Y.L., H.J., J.K. and H.C. acknowledge the support by the National Research Foundation of Korea Grant funded by the Korean Government (no. 2019R1A2C3006189). K.W. and T.T. acknowledge the support from the Japan Society for the Promotion of Science, KAKENHI (grant nos. 19H05790, 20H00354 and 21H05233) and from A3 Foresight by the Japan Society for the Promotion of Science. Support for P.Y.H. was provided by the Illinois Materials Research Science and Engineering Center through the National Science Foundation MRSEC programme (award no. DMR-1720633). G.-H.L. acknowledges the support from the Research Institute of Advanced Materials, Institute of Engineering Research, Institute of Applied Physics and Inter-University Semiconductor Research Center at Seoul National University.
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J.-H.B. and G.-H.L. designed and conceived the project. H.G.K., Y.C. and M.K. performed TEM and HAADF–STEM imaging. S.Y.L., H.J., J.K. and H.C. performed PL measurements at low temperature. H.R. fabricated samples for PL measurement. S.C.H. and Y.J. synthesized TMDs by CVD. Y.Z. and P.Y.H. discussed TEM and STEM results. K.W. and T.T. supplied boron nitride crystals. J.-H.B. and G.-H.L. jointly analysed the data and wrote the paper.
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Baek, JH., Kim, H.G., Lim, S.Y. et al. Thermally induced atomic reconstruction into fully commensurate structures of transition metal dichalcogenide layers. Nat. Mater. 22, 1463–1469 (2023). https://doi.org/10.1038/s41563-023-01690-2
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DOI: https://doi.org/10.1038/s41563-023-01690-2
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