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A Gd@C82 single-molecule electret

Abstract

Electrets are dielectric materials that have a quasi-permanent dipole polarization. A single-molecule electret is a long-sought-after nanoscale component because it can lead to miniaturized non-volatile memory storage devices. The signature of a single-molecule electret is the switching between two electric dipole states by an external electric field. The existence of these electrets has remained controversial because of the poor electric dipole stability in single molecules. Here we report the observation of a gate-controlled switching between two electronic states in Gd@C82. The encapsulated Gd atom forms a charged centre that sets up two single-electron transport channels. A gate voltage of ±11 V (corresponding to a coercive field of ~50 mV Å–1) switches the system between the two transport channels with a ferroelectricity-like hysteresis loop. Using density functional theory, we assign the two states to two different permanent electrical dipole orientations generated from the Gd atom being trapped at two different sites inside the C82 cage. The two dipole states are separated by a transition energy barrier of 11 meV. The conductance switching is then attributed to the electric-field-driven reorientation of the individual dipole, as the coercive field provides the necessary energy to overcome the transition barrier.

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Fig. 1: Single-electron transport of the Gd@C82 SMD.
Fig. 2: Gate-controlled switching between the two molecular states showing a ferroelectricity-like hysteresis loop.
Fig. 3: Simulating a two-resistance-state operation based on the SMD switching.
Fig. 4: Density functional theory calculations revealing the SME physics.

Data availability

The data shown in the paper are available at https://doi.org/10.6084/m9.figshare.12720392. Source data are provided with this paper.

Code availability

The density functional theory program used to analyse the results is available from the corresponding author on reasonable request.

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Acknowledgements

We gratefully acknowledge the financial support of the National Key R&D Program of China (2017YFA0303203, 2018YFE0202700, 2018YFA0306004 and 2016YFA0300101), the National Natural Science Foundation of China (U1732273, 21973038, 91961101, 61761166009, 11522432, 11574217, U1732159, 61822403, 11874203, 11904166, 11622437, 61674171, 11974422, 21721001, 91961112, 11227904, 61521001 and 61801209), the Strategic Priority Research Program of Chinese Academy of Sciences (grant no. XDB30000000), the Fundamental Research Funds for the Central Universities, China, and the Research Funds of Renmin University of China (grants no. 16XNLQ01 and 19XNQ025), the Fundamental Research Funds for the Central Universities (020414380082, 020414380127, 020414380150 and 020414380151) and the opening Project of the Wuhan National High Magnetic Field Center. C.W. was supported by the Outstanding Innovative Talents Cultivation Funded Programs 2017 of Renmin University of China. Calculations were performed at the Physics Lab of High-Performance Computing of Renmin University of China and Shanghai Supercomputer Center. S.-F.S. acknowledges support from NSF Career Grant DMR-1945420 and NYSTAR through Focus Center-NY–RPI contract C150117. We thank H.-L. Cai from Nanjing University for stimulating discussions. We also thank S.-T. Zhang from Nanjing University for preparing bulk materials.

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F.S. conceived the research and B.W., W.J., S.-Y.X., S.-F.S. and M.A.R. co-supervised the project. M.Z. performed the bulk material measurements. C.W. and W.J. performed and analysed the density functional theory calculations. Z.B. designed and fabricated the devices. K.Z. performed the SMD measurements. F.-F.X. performed high-performance liquid chromatography for purification of the molecular materials. Y.-Z.T. participated in the separation of the molecular materials. S.-Y.X. prepared the molecular materials. X.T. and D.P. assisted in the device fabrication. Y.G. and J.W. assisted with the density functional theory calculations. K.Z., C.W., F.S., W.J. and M.A.R. wrote the paper. K.-J.H., L.C., S.Z., L.K., J.C., P.W., X.W., J.L., Y.S. and G.W. participated in discussions on this manuscript. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Fengqi Song or Wei Ji or Su-Yuan Xie or Su-Fei Shi or Mark A. Reed.

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Peer review information Nature Nanotechnology thanks Sadafumi Nishihara and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Zhang, K., Wang, C., Zhang, M. et al. A Gd@C82 single-molecule electret. Nat. Nanotechnol. 15, 1019–1024 (2020). https://doi.org/10.1038/s41565-020-00778-z

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