Abstract
Recent work investigated graphene’s hydrogenation with independent control of the electric field, E, and charge density, n, in the crystal and showed that the process is controlled by n. Here, we demonstrate layer-selective conductor–insulator transitions in twisted bilayer graphene, driven by hydrogenation at fixed n under strong E. This process is accompanied by proton transport through the bilayer, enabling several parallel and configurable logic gates in the devices. Selectivity arises because the large twist angle decouples the two layers’ electronic systems, enabling independent control of their charge densities. Polarisation by the field then induces a charge imbalance at fixed total n, triggering hydrogenation when one of the layers’ charge densities reaches the threshold for monolayer hydrogenation. Our results introduce a new type of electrode-electrolyte interface in which electrochemical processes are controlled with two decoupled 2D electron gases, opening new design opportunities for energy and information processing devices.
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Acknowledgements
This work was supported by UKRI (EP/X017745: M.L.-H, EP/X041204: S.J.H., EP/S021531: S.S-S., EP/Y024303:G.T.), the Directed Research Projects Program of the Research and Innovation Center for Graphene and 2D Materials at Khalifa University (RIC2D-D001: M.L.-H., L.F.V. and D.B.), The Royal Society (URF\R1\201515: M.L.-H.), the U.S. Army DEVCOM ARL Army Research Office (ARO) Energy Sciences Competency, (Electrochemistry or Advanced Energy Materials) Program award # W911NF-25-1-0041 (M.L-H.). The views and conclusions contained in this document are those of the authors and should not be interpreted as representing the official policies, either expressed or implied, of the U.S. Army or the U.S. Government. Part of this work was supported by the Flemish Science Foundation (FWO-Vl: F.M.P.) and FUNCAP and CNPq (312539/2025-8, 437067/2018-1, 423423/2021-5, 408144/2022-0: RNCF), and the European Research Council (Grant ERC-2016-STG-EvoluTEM-715502, S.J.-H.). TEM access was supported by the Henry Royce Institute for Advanced Materials, funded through EPSRC grants EP/R00661X, EP/S019367, EP/P025021 and EP/P025498.
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M.L.-H. designed and directed the project with J.T. J.T., G.C., E.H., M.A., X.Z. & Y.M. fabricated devices. J.T. & H.L. performed the transport measurements and analysis with help from D.D and E.H. G.R.T., S.S.-A. & S.J.H. performed STEM characterisation and analysis. F.M.P. and D. R. C. performed analytical theory calculations. D.B. & L.F.V. performed DFT calculations. M.L.-H. & J.T. wrote the manuscript with input from all the authors.
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Tong, J., Chen, G., Li, H. et al. Layer-selective hydrogenation and proton transport in twisted bilayer graphene. Nat Commun (2026). https://doi.org/10.1038/s41467-026-71147-y
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DOI: https://doi.org/10.1038/s41467-026-71147-y
