Abstract
Atomically thin van der Waals (vdW) films provide a material platform for the epitaxial growth of quantum heterostructures. However, unlike the remote epitaxial growth of three-dimensional bulk crystals, the growth of two-dimensional material heterostructures across atomic layers has been limited due to the weak vdW interaction. Here we report the double-sided epitaxy of vdW layered materials through atomic membranes. We grow vdW topological insulators Sb2Te3 and Bi2Se3 by molecular-beam epitaxy on both surfaces of atomically thin graphene or hexagonal boron nitride, which serve as suspended two-dimensional vdW substrate layers. Both homo- and hetero-double-sided vdW topological insulator tunnel junctions are fabricated, with the atomically thin hexagonal boron nitride acting as a crystal-momentum-conserving tunnelling barrier with abrupt and epitaxial interfaces. By performing field-angle-dependent magneto-tunnelling spectroscopy on these devices, we reveal the energy–momentum–spin resonance of massless Dirac electrons tunnelling between helical Landau levels developed in the topological surface states at the interfaces.
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The data that support the findings of this study are presented in the Article and its Extended Data. Further data are available from the corresponding authors upon reasonable request.
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Acknowledgements
We thank J. Eom, Y. S. Kim and C.-H. Lee for their assistance with transferring atomically thin vdW crystals onto perforated SiNx membranes. We also express our gratitude to S. Cho and Effucell for providing technical support with the UHV MBE system. Additionally, we thank J. S. Lee of the National Center for Inter-University Research Facilities at Seoul National University for assistance with the focused ion beam system. The major part of this work was supported by the Office of Naval Research (ONR) Multidisciplinary University Research Initiatives (MURI) program (N00014-21-1-2377) and the Science Research Center (SRC) for Novel Epitaxial Quantum Architectures (NRF-2021R1A5A1032996). J.Y.P. and P.K. acknowledge support from ONR (N00014-24-1-2081). J.S., J.K. and D.K. acknowledge support from the National Research Foundation of Korea (NRF) grants funded by the Korean Government (grant nos. RS-2023-00283291, RS-2023-00207732 and 2023R1A2C2005809). J.J. and M.K. acknowledge support from the NRF (NRF-2022R1A2C3007807). H.Y. acknowledges support from the NRF (grant nos. 2021R1C1C1010924 and 2020R1F1A1049563). H.S.S. acknowledges support from the Institute for Basic Science (IBS-R036-D1). A portion of the user collaboration grant program (UCGP) project was performed at the National High Magnetic Field Laboratory supported by the National Science Foundation through NSF/DMR-1644779 and the State of Florida. K.W. and T.T. acknowledge support from the JSPS KAKENHI (grant nos. 20H00354 and 23H02052) and World Premier International Research Center Initiative (WPI), MEXT, Japan.
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Contributions
P.K., G.-C.Y. and J.Y.P. conceived the experiments. J.Y.P. performed the double-sided vdW epitaxy and fabricated the tunnelling devices. J.Y.P. and G.-C.Y. analysed and optimized these processes. J.Y.P. performed the magneto-tunnelling measurements together with J.S. and J.K. J.Y.P., R.M.H., A.G. and W.K.P. carried out the measurements at the National High Magnetic Field Laboratory. J.Y.P., J.S., J.K., D.K. and P.K. analysed the transport data. J.J. conducted the TEM experiments. J.J., J.Y.P., G.-C.Y. and M.K. analysed the TEM data. J.Y.P. and H.Y. prepared the hole-patterned SiNx membrane templates. Y.J.S., D.H., H.Y. and J.Y.P. carried out the suspension of ultrathin vdW layers on the perforated SiNx membranes. C.H. and H.S.S. provided the epitaxial few-layer hBN films and collaborated on discussions about the double-sided vdW epitaxy on them. J.Y. grew the monolayer graphene. K.W. and T.T. provided the bulk hBN single crystals. G.-C.Y. and P.K. jointly supervised the project. J.Y.P. and P.K. wrote the manuscript with input from all authors.
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Extended data
Extended Data Fig. 1 Suspension of atomically thin hBN crystals on the perforated SiNx membrane.
a–c, Optical microscope images of ultrathin hBN layers: as exfoliated on the SiO2 surface (a), picked up by the PCL polymer stamp (b), transferred on the SiNx membrane with premade holes (c).
Extended Data Fig. 2 Lateral overgrowth of the bottom TI layer.
Cross-sectional schematic illustration (a; not drawn to scale) and scanning electron microscopy image (b; 52° tilted view) of the sample shown in Fig. 3a, depicting the lateral overgrowth of the bottom TI layer at the hBN(graphene)/SiNx interface and the bottom edge of the hole in the SiNx membrane. This is due to lateral diffusion of adatoms at the vdW terminated growth front, resulting in highly anisotropic growth that favors lateral over vertical growth. The growth rate is slower at the bottom of the suspended vdW layer due to the shadowing effect of the TI films laterally grown over the bottom edge of the hole in the SiNx.
Extended Data Fig. 3 Larger scale homogeneity of the Bi2Se3/hBN/Bi2Se3 interface.
Cross-sectional HR-TEM images of Bi2Se3/2 ML hBN/Bi2Se3 taken along the zone axis [\(1\bar{2}10\)] exhibiting atomically sharp and clean interfaces.
Extended Data Fig. 4 Epitaxial relationship of the TI thin films grown on a single surface of suspended graphene substrates.
a–c, Plan-view SAED patterns of the Bi2Se3 thin film grown on the top surface of suspended graphite (a), the Bi2Se3 thin film grown on the bottom surface of suspended monolayer graphene (b), and the Sb2Te3 thin film grown on the top surface of suspended monolayer graphene (c). Insets: Plan-view TEM BF images. The white solid circles and the yellow dashed circles indicate the areas in which the SAED in the corresponding main panels are taken and the suspended regions, respectively. The entire area displayed in the inset is suspended for a. Scale bars in the insets: 1 μm (a), 200 nm (b), and 200 nm (c). All data (a–c) exhibit the preferential epitaxial relationship of \({\{10\bar{1}0\}}_{{{\rm{Bi}}}_{2}{{\rm{Se}}}_{3}\,{{\rm{or}}\,{\rm{Sb}}}_{2}{{\rm{Te}}}_{3}}\parallel {\{10\bar{1}0\}}_{{\rm{graphene}}\,{\rm{or}}\,{\rm{graphite}}}\), indicating that the epitaxial alignment in the double-sided vdW epitaxy is owing to the local interaction at the interface with the suspended vdW substrate layer.
Extended Data Fig. 5 Tunneling device fabrication processes.
a, Optical microscope image of atomically thin hBN layers suspended on the perforated SiNx membrane. Inset: High-contrast image of the main panel. Scale bar: 10 μm. b, Optical microscope image of the sample in (a) after the double-sided vdW epitaxy of TI thin films (10 QL Bi2Se3 on the back side and 20 QL Sb2Te3 on the top side). c, Photograph (upper left) and schematic (lower right) of the double-sided vdW epitaxial heterojunction after the evaporation of the Ti/Au 5/200 nm common bottom contact. d,e, Optical microscope images of the junction arrays: after the fabrication of Ti/Au 5/55 nm individual top contacts followed by Ar plasma etching (d) and after the formation of bonding pads and leads (Ti/Pd/Au 5/20/125 nm). f, Optical microscope image (upper left) and schematic structure (lower right) of the finished device.
Extended Data Fig. 6 Magnetic field-dependent tunnelling conductance of a Bi2Se3/3 ML hBN/Bi2Se3 device.
a, Differential conductance \(G(V)=\partial I/\partial V\) of the Bi2Se3/3 ML hBN/Bi2Se3 device at zero magnetic field. b–d, Colour scale maps showing the field-modulated component of the conductance ΔG(V, B) at different field angles: out-of-plane (b), 45° tilted (c), and in-plane (d) directions. B⟂ and B∥ components of the field are indicated by the left and right ticks, respectively. The black dashed horizontal line in b indicates the maximum B⟂ in c. We observe oscillatory features that develop at higher B⟂, with their peak and valley positions varying as a function of B⟂, in addition to the field-angle-independent oscillatory features arising from the bulk QWSs. We are however unable to conclusively identify conductance oscillations associated with the LL formation in TSSs, presumably because the conductance is dominated by the bulk-to-bulk tunnelling as both the b- and t-Bi2Se3 films are degenerately n-doped. The difference in thickness between the b-Bi2Se3 (10 QL) and t-Bi2Se3 (20 QL) is responsible for the asymmetry in the periodicity of the QWS-related oscillations at negative and positive biases. All measurements are performed at T = 0.3 K.
Extended Data Fig. 7 Temperature dependence of tunnelling current and tunnelling conductance.
a,b, Tunnelling current I(V) (a) and differential conductance G(V) = ∂I/∂V (b) of Bi2Se3/3 ML hBN/Sb2Te3 device at different temperatures. Inset: Zero-bias differential conductance G(V = 0) as a function of temperature. The NDC behaviour is enhanced as temperature decreases, consistent with the broken-gap energy band alignment picture35. The bulk-originated oscillatory features (V < 0) and the local maximum in G (V ~0.22 V) become evident at T ≤ 7 K of our data.
Extended Data Fig. 8 Oscillations in the tunnelling conductance associated with the bulk QWSs.
Differential conductance \(G(V)=\partial I/\partial V\) of the Bi2Se3/2 ML hBN/Sb2Te3 device at zero magnetic field (black) and B∥ = 14 T (red). The inset shows \(\partial G/\partial V={\partial }^{2}I/{\partial V}^{2}\) as a function of V at different B∥, obtained by taking numerical derivative of G(V). The black arrows indicate the positions of the peaks of the oscillatory feature (1) related to the bulk QWSs, appearing in ΔG(V, B) (Fig. 4b–e). One can find that they correspond to the valleys of the QWS resonances in G(V, B = 0), which become smoothened out at higher B∥ as fine structures develop due to the Zeeman effects. The G(V, B = 0) peak at V = 225 mV, attributed to the alignment of the bulk band edges, is also suppressed at higher B∥ by the Zeeman effects. All data is measured at T = 1.8 K.
Extended Data Fig. 9 LL peak identifications and LL index assignments.
a, Field-modulated component of the tunnelling conductance ΔG(V, B) at θ = 0° and T = 1.8 K, the same data as Fig. 4b replotted with \({B}_{\perp }^{1/2}\) as the vertical axis so that the LLs formed in the Dirac states appear as linear lines, ignoring the Zeeman energy. b, Peaks identified in a. The lime-coloured dots represent the peak positions identified by MATLAB’s findpeaks function, a tool for locating local maxima, applied along the vertical and horizontal axes, as well as in two diagonal directions. The transparency of the dots corresponds to the prominence of the peaks the function returns. c, LL index assignments. The positions of the peaks assigned to each LL index n are indicated by the corresponding colour. The green dots are the positions of the peaks not associated with the LLs. The solid lines tracing the peaks corresponding to n < 0 (red) and n > 0 (blue) LLs of Sb2Te3, and the inter-band inter-LL resonant tunneling between Bi2Se3 and Sb2Te3 (magenta) are reconstructed from the slopes and intercepts of the linear fits in Fig. 4f. The dark grey curve is a fit to the n = 0 LL peaks shifting linearly with respect to B⟂. The dotted curve and line trace the n = 0′ and 1′ LL peaks of unclear origin, respectively.
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Park, J.Y., Shin, Y.J., Shin, J. et al. Double-sided van der Waals epitaxy of topological insulators across an atomically thin membrane. Nat. Mater. 24, 399–405 (2025). https://doi.org/10.1038/s41563-024-02079-5
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DOI: https://doi.org/10.1038/s41563-024-02079-5
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