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Room-temperature logic-in-memory operations in single-metallofullerene devices

Nature Materials volume 21, pages 917–923 (2022)Cite this article

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Abstract

In-memory computing provides an opportunity to meet the growing demands of large data-driven applications such as machine learning, by colocating logic operations and data storage. Despite being regarded as the ultimate solution for high-density integration and low-power manipulation, the use of spin or electric dipole at the single-molecule level to realize in-memory logic functions has yet to be realized at room temperature, due to their random orientation. Here, we demonstrate logic-in-memory operations, based on single electric dipole flipping in a two-terminal single-metallofullerene (Sc2C2@Cs(hept)-C88) device at room temperature. By applying a low voltage of ±0.8 V to the single-metallofullerene junction, we found that the digital information recorded among the different dipole states could be reversibly encoded in situ and stored. As a consequence, 14 types of Boolean logic operation were shown from a single-metallofullerene device. Density functional theory calculations reveal that the non-volatile memory behaviour comes from dipole reorientation of the [Sc2C2] group in the fullerene cage. This proof-of-concept represents a major step towards room-temperature electrically manipulated, low-power, two-terminal in-memory logic devices and a direction for in-memory computing using nanoelectronic devices.

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Fig. 1: The mechanism of the single-metallofullerene memory device.
Fig. 2: Single-molecule conductance measurements and the in situ two-conductance-state switching and storage operations of single-Sc2C2@Cs(hept)-C88 devices.
Fig. 3: Boolean logic operations in single-metallofullerene devices of Sc2C2@Cs(hept)-C88.
Fig. 4: The two-state memristive mechanism of Sc2C2@Cs(hept)-C88.

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Data availability

The authors declare that the main data supporting the findings of this study are available within this article and its Supplementary Information. Source data are provided with this paper. Extra data are available from the corresponding authors upon request.

Code availability

The data analysis of conductance measurements was performed using our open-source code XME analysis, which is available at https://github.com/Pilab-XMU/XMe_DataAnalysis. The computation details can be made available from the corresponding authors upon request.

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Acknowledgements

This work was supported by the National Key R&D Programme of China (grant no. 2017YFA0204902 (W.H.)), the National Natural Science Foundation of China (grant nos. 92061204 (S.-Y.X.), 21933012 (J.-Y.L.), 31871877 (J.-Y.L.), 21973079 (Y.Y.), 22032004 (Y.Y.) and 21721001 (S.-Y.X.)), the Fundamental Research Funds for the Central Universities (grant no. 20720200068 (J.-Y.L.)), the UK EPSRC (grant nos. EP/M014452/1 (C.J.L.), EP/P027156/1 (C.J.L.) and EP/N03337X/1 (C.J.L.)). We thank J. Wang and L. Huang for their help with the STM-BJ equipment in the glove box.

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Author notes

  1. These authors contributed equally: Jing Li, Songjun Hou, Yang-Rong Yao, Chengyang Zhang.

Authors and Affiliations

  1. State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering and Institute of Artificial Intelligence and Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen University, Xiamen, China

    Jing Li, Yang-Rong Yao, Chengyang Zhang, Hai-Chuan Wang, Hewei Zhang, Xinyuan Liu, Chun Tang, Mengxi Wei, Wei Xu, Yaping Wang, Jueting Zheng, Zhichao Pan, Junyang Liu, Jia Shi, Yang Yang, Su-Yuan Xie & Wenjing Hong

  2. Department of Physics, Lancaster University, Lancaster, UK

    Songjun Hou, Qingqing Wu & Colin J. Lambert

  3. Key Laboratory of Multifunctional Nanomaterials and Smart Systems, Division of Advanced Materials, Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences, Suzhou, China

    Lixing Kang

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Contributions

W.H., S.-Y.X. and J.L. conceived the idea for the paper. Y.-R.Y and S.-Y.X. synthesized and characterized the endohedral metallofullerene molecules. J.Z. fabricated the mechanically controllable break junction chips. J.L., H.-C.W., X.L., J.S., C.Z. and J.Z. measured the conductance, conductance–voltage and characterization of the in situ logic operation. S.H., Q.W. and C.J.L. conducted the theoretic calculations. J.L., H.Z., Y.W. and C.Z. discussed and produced the picture. C.T., M.W., J.-Y.L., W.X. and Y.Y. helped to discuss the mechanism. Z.P. and L.K. supported the data analysis. J.L., S.H., Q.W., C.J.L., S.-Y.X. and W.H. analysed and discussed the data and wrote the paper.

Corresponding authors

Correspondence to Colin J. Lambert, Su-Yuan Xie or Wenjing Hong.

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Nature Materials thanks Andrew Briggs and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–25, Discussion and Table 1.

Supplementary Data 1

The raw ultraviolet–visible, mass data and GV data.

Supplementary Data 1

Two-state-switching and logic-in-memory operation data.

Supplementary Data 1

Charge transport and computation data.

Source data

Source Data Fig. 2

Statistical source data.

Source Data Fig. 3

Statistical source data.

Source Data Fig. 4

Computation data

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Li, J., Hou, S., Yao, YR. et al. Room-temperature logic-in-memory operations in single-metallofullerene devices. Nat. Mater. 21, 917–923 (2022). https://doi.org/10.1038/s41563-022-01309-y

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