Abstract
In situ tailoring of two-dimensional materials’ phases under external stimulus facilitates the manipulation of their properties for electronic, quantum and energy applications. However, current methods are mainly limited to the transitions among phases with unchanged chemical stoichiometry. Here we propose on-device phase engineering that allows us to realize various lattice phases with distinct chemical stoichiometries. Using palladium and selenide as a model system, we show that a PdSe2 channel with prepatterned Pd electrodes can be transformed into Pd17Se15 and Pd4Se by thermally tailoring the chemical composition ratio of the channel. Different phase configurations can be obtained by precisely controlling the thickness and spacing of the electrodes. The device can be thus engineered to implement versatile functions in situ, such as exhibiting superconducting behaviour and achieving ultralow-contact resistance, as well as customizing the synthesis of electrocatalysts. The proposed on-device phase engineering approach exhibits a universal mechanism and can be expanded to 29 element combinations between a metal and chalcogen. Our work highlights on-device phase engineering as a promising research approach through which to exploit fundamental properties as well as their applications.
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Data availability
The main data supporting the findings of this study are available within the paper and its Supplementary Information. Additional data are available from the corresponding authors upon reasonable request. Source data are provided with this paper.
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Acknowledgements
This work was supported in part by the National Key R&D Program of China under grants 2023YFF1203600 (S.-J.L.) and 2022YFA1402500 (J.S.); the National Natural Science Foundation of China (62122036 (S.-J.L.), 62034004 (F.M.), 61921005 (F.M.), 62204112 (J.S.), 12074176 (B.C.), 12104206 (L.Z.) and 11974156 (J.L.)); the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB44000000 (F.M.)); the Leading-edge Technology Program of Jiangsu Natural Science Foundation (BK20232004 (F.M.)); the Natural Science Foundation of Jiangsu Province (BK20220774 (J.S.)); the Guangdong Innovative and Entrepreneurial Research Team Program (2019ZT08C044 (J.L.)); the Shenzhen Science and Technology Program (20200925161102001 (J.L.) and 20210609103649046 (J.L.)); the Science, Technology and Innovation Commission of Shenzhen Municipality (ZDSYS20190902092905285 (J.L.)); and the Quantum Science Strategic Special Project from the Quantum Science Center of the Guangdong-Hong Kong-Macao Greater Bay Area (GDZX2301006 (J.L.)). STEM characterization was performed at the Pico Center from SUSTech Core Research Facilities, which receives support from the Presidential Fund and Development and Reform Commission of Shenzhen Municipality. F.M. and S.-J.L. acknowledge support from the AIQ Foundation and the e-Science Center of the Collaborative Innovation Center of Advanced Microstructures. We also acknowledge the microfabrication center of the National Laboratory of Solid State Microstructures (NLSSM) for their technical support.
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S.-J.L. and F.M. conceived the idea. S.-J.L. and F.M. supervised the whole project. X. Liu, J.S. and T.C. fabricated devices and performed electrical and Raman measurements. L.Z., G.W., Q.Y. and J.L. performed the electron microscopy experiments and data analysis. J.M. and X. Luo carried out the DFT calculations and data analysis. J.S., Z.S., M.M. and Y.H. carried out the measurements of electrocatalytic performance. J.S. and Z.L. carried out the measurements of contact resistance. X. Liu, S.Y. and L.W. grew the materials. J.S., Y.D., J.X., F.C., B.W., C.P. and B.C. assisted in device processing and characterization. Z.W. assisted in the Raman characterization. X. Liu, J.S., S.-J.L. and F.M. wrote the manuscript with input from all authors.
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Liu, X., Shan, J., Cao, T. et al. On-device phase engineering. Nat. Mater. (2024). https://doi.org/10.1038/s41563-024-01888-y
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DOI: https://doi.org/10.1038/s41563-024-01888-y
