Abstract
Zero-dimensional quantum dots (QDs), which have inherent quantum confinement effects and sharp discrete energy levels, are regarded as essential building blocks for quantum information devices. Current manufacturing strategies often exhibit limited adaptability in terms of compositional design or interface engineering. Here we propose a van der Waals (vdW) epitaxial strategy for growing intrinsic QDs by modulating the interfacial couplings between vdW surfaces and QDs. Versatile III–V (MX, M = Ga, In; X = As, Sb) and IV–VI (SnTe) QDs were fabricated without considering the lattice mismatch constraints, leading to QDs with more intrinsic features. We further demonstrated that the as-grown InSb QDs/MoS2 showed a broadened photoresponse in the near-infrared region due to the efficient charge-transfer channels at their vdW interfaces. This work reports a synthetic route to the all-in-solid epitaxy of QDs, which may expand the optoelectronic applications of QDs beyond those that are conventionally grown.
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Acknowledgements
This work was financially supported by the National Natural Science Foundation of China (grant numbers 62222408 (to S.Z.), 62125404 (to Z.W.), 12274404 (to S.Z.), 62375256 (to J.Y.), 52322205 (to C.L.), 52250398 (to C.L.) and 12274456 (to C.L.)), in part by the Youth Innovation Promotion Association of the Chinese Academy of Sciences (grant number 2022112 (to S.Z.)), the Beijing Natural Science Foundation (grant number Z220005 (to Z.W.)), the National Key Research and Development Program of China (grant numbers 2020YFB1506400 (to Z.W.) and 2022YFA1405600 (to C.L.)), the Strategic Priority Research Program of Chinese Academy of Sciences (grant number XDB43000000 (to Z.W.) and XDB0460000 (to H.-X.D.)), and the CAS Project for Young Scientists in Basic Research (grant number YSBR-026 (to Z.W.)).
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S.Z., Z.W., F.L. and C.L. supervised the project. K.X., L.L. and Z.Z. conducted the sample growth and characterizations. K.X. and Z.Z. wrote the article. C.Z. performed the theoretical calculations. J.Y., H.-X.D., J.Z., J.L. and K.L. revised the manuscript. All the authors discussed the results and commented on the manuscript.
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Nature Synthesis thanks Chen Shang and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.
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Extended data
Extended Data Fig. 1 Schematics of QDs grown by vdW epitaxy and coherent epitaxy.
a, The non-layered stable phase tends to reduce the surface energy, hence forming QDs with large aspect ratios on vdW substrates. b, Typical coherent epitaxy commonly requires a wetting layer to accumulate stress followed by strain release to form QDs.
Extended Data Fig. 2 InAs QDs grown on wafer-scale FL mica with highly uniform distribution of size and density.
a, Photograph of a 2-inch FL mica on which InAs QDs were grown. b, AFM images of InAs QDs grown on the 2-inch FL mica wafer at nine positions denoted by the red dots. The insets show the magnified views of InAs QDs at the centre square with 200 nm sides of each position (80 μm×80 μm).
Extended Data Fig. 3 Regulation of the QD size and density by substrate temperature and growth time.
a-f, InAs QDs grown on FL mica at 200 °C, 220 °C, 250 °C, 280 °C, 310 °C, and 340 °C for 1 min, leading to densities of 1.6×1011 cm−2, 2.5×1010 cm−2, 1.0×109 cm−2, 2.4×108 cm−2, 4.0×107 cm−2, and 2.5×107 cm−2, respectively. g-i, InAs QDs grown on FL mica at 280 °C for 30 s, 3 min, and 5 min, leading to average sizes of 10 nm, 20 nm, and 50 nm, respectively.
Extended Data Fig. 4 Epitaxial relationship between InAs QDs and FL mica.
a, Cross-sectional high-resolution transmission electron microscopy (HRTEM) image of a series of InAs QDs on FL mica. b-d, Three magnified views of InAs QDs with lattice configuration of InAs-(111) contacting the vdW surface of FL mica.
Supplementary information
Supplementary Information
Supplementary Figs. 1–9 and Note 1.
Supplementary Data 1
Source data for Supplementary Fig. 1.
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Supplementary Data 3
Numerical experimental data for Supplementary Fig. 6.
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Xin, K., Li, L., Zhou, Z. et al. Epitaxial growth of quantum dots on van der Waals surfaces. Nat. Synth 3, 1176–1183 (2024). https://doi.org/10.1038/s44160-024-00562-0
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DOI: https://doi.org/10.1038/s44160-024-00562-0
