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Observation of single-defect memristor in an MoS2 atomic sheet

Abstract

Non-volatile resistive switching, also known as memristor1 effect, where an electric field switches the resistance states of a two-terminal device, has emerged as an important concept in the development of high-density information storage, computing and reconfigurable systems2,3,4,5,6,7,8,9. The past decade has witnessed substantial advances in non-volatile resistive switching materials such as metal oxides and solid electrolytes. It was long believed that leakage currents would prevent the observation of this phenomenon for nanometre-thin insulating layers. However, the recent discovery of non-volatile resistive switching in two-dimensional monolayers of transition metal dichalcogenide10,11 and hexagonal boron nitride12 sandwich structures (also known as atomristors) has refuted this belief and added a new materials dimension owing to the benefits of size scaling10,13. Here we elucidate the origin of the switching mechanism in atomic sheets using monolayer MoS2 as a model system. Atomistic imaging and spectroscopy reveal that metal substitution into a sulfur vacancy results in a non-volatile change in the resistance, which is corroborated by computational studies of defect structures and electronic states. These findings provide an atomistic understanding of non-volatile switching and open a new direction in precision defect engineering, down to a single defect, towards achieving the smallest memristor for applications in ultra-dense memory, neuromorphic computing and radio-frequency communication systems2,3,11.

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Fig. 1: Material characterization.
Fig. 2: Atomistic characterization of MoS2 monolayers.
Fig. 3: Atomistic observation of ‘set–reset’ sequences for VS2 defects.
Fig. 4: Atomistic defect simulations and spectral calculations for monolayer MoS2.

Data availability

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

References

  1. Chua, L. Memristor-the missing circuit element. IEEE Trans. Circuit Theory 18, 507–519 (1971).

    Article  Google Scholar 

  2. Wong, H.-S. P. & Salahuddin, S. Memory leads the way to better computing. Nat. Nanotechnol. 10, 191–194 (2015).

    Article  CAS  Google Scholar 

  3. Akinwande, D. et al. Graphene and two-dimensional materials for silicon technology. Nature 573, 507–518 (2019).

    Article  CAS  Google Scholar 

  4. Wouters, D. J., Waser, R. & Wuttig, M. Phase-change and redox-based resistive switching memories. Proc. IEEE 103, 1274–1288 (2015).

    Article  CAS  Google Scholar 

  5. Zhao, H. et al. Atomically thin femtojoule memristive device. Adv. Mater. 29, 1703232 (2017).

    Article  Google Scholar 

  6. Wang, M. et al. Robust memristors based on layered two-dimensional materials. Nat. Electron. 1, 130–136 (2018).

    Article  CAS  Google Scholar 

  7. Xu, R. et al. Vertical MoS2 double-layer memristor with electrochemical metallization as an atomic-scale synapse with switching thresholds approaching 100 mV. Nano Lett. 19, 2411–2417 (2019).

    Article  CAS  Google Scholar 

  8. Zhang, F. et al. Electric-field induced structural transition in vertical MoTe2- and Mo1-xWxTe2-based resistive memories. Nat. Mater. 18, 55–61 (2019).

    Article  CAS  Google Scholar 

  9. Sangwan, V. K. et al. Gate-tunable memristive phenomena mediated by grain boundaries in single-layer MoS2. Nat. Nanotechnol. 10, 403–406 (2015).

    Article  CAS  Google Scholar 

  10. Ge, R. et al. Atomristor: nonvolatile resistance switching in atomic sheets of transition metal dichalcogenides. Nano Lett. 18, 434–441 (2017).

    Article  Google Scholar 

  11. Kim, M. et al. Zero-static power radio-frequency switches based on MoS2 atomristors. Nat. Commun. 9, 2524 (2018).

    Article  Google Scholar 

  12. Wu, X. et al. Thinnest nonvolatile memory based on monolayer h‐BN. Adv. Mater. 31, 1806790 (2019).

    Article  Google Scholar 

  13. Ge, R. et al. Atomristors: memory effect in atomically-thin sheets and record RF switches. Proc. IEEE International Electron Devices Meeting (IEDM) 22.6.1–22.6.4 (2018).

  14. Valov, I., Waser, R., Jameson, J. R. & Kozicki, M. N. Electrochemical metallization memories—fundamentals, applications, prospects. Nanotechnology 22, 254003 (2011).

    Article  Google Scholar 

  15. Velicky, M. J. et al. Mechanism of gold-assisted exfoliation of centimeter-sized transition-metal dichalcogenide monolayers. ACS Nano 12, 10463–10472 (2018).

    Article  CAS  Google Scholar 

  16. Liu, Z. et al. Strain and structure heterogeneity in MoS2 atomic layers grown by chemical vapour deposition. Nat. Commun. 5, 5246 (2014).

    Article  Google Scholar 

  17. Vancsó, P. et al. The intrinsic defect structure of exfoliated MoS2 single layers revealed by scanning tunneling microscopy. Sci. Rep. 6, 29726 (2016).

    Article  Google Scholar 

  18. González, C., Biel, B. & Dappe, Y. J. Theoretical characterisation of point defects on a MoS2 monolayer by scanning tunnelling microscopy. Nanotechnology 27, 105702 (2016).

    Article  Google Scholar 

  19. Zhou, W. et al. Intrinsic structural defects in monolayer molybdenum disulfide. Nano Lett. 13, 2615–2622 (2013).

    Article  CAS  Google Scholar 

  20. Zhang, C., Johnson, A., Hsu, C.-L., Li, L.-J. & Shih, C.-K. Direct imaging of band profile in single layer MoS2 on graphite: quasiparticle energy gap, metallic edge states, and edge band bending. Nano Lett. 14, 2443–2447 (2014).

    Article  CAS  Google Scholar 

  21. Sørensen, S. G., Füchtbauer, H. G., Tuxen, A. K., Walton, A. S. & Lauritsen, J. V. Structure and electronic properties of in situ synthesized single-layer MoS2 on a gold surface. ACS Nano 8, 6788–6796 (2014).

    Article  Google Scholar 

  22. Zhou, X. et al. Periodic modulation of the doping level in striped MoS2 superstructures. ACS Nano 10, 3461–3468 (2016).

    Article  CAS  Google Scholar 

  23. Chiu, M.-H. et al. Determination of band alignment in the single-layer MoS2/WSe2 heterojunction. Nat. Commun. 6, 7666 (2015).

    Article  CAS  Google Scholar 

  24. Martinez-Castro, J. et al. Scanning tunneling microscopy of an air sensitive dichalcogenide through an encapsulating layer. Nano Lett. 18, 6696–6702 (2018).

    Article  CAS  Google Scholar 

  25. Song, S. H., Joo, M.-K., Neumann, M., Kim, H. & Lee, Y. H. Probing defect dynamics in monolayer MoS2 via noise nanospectroscopy. Nat. Commun. 8, 2121 (2017).

    Article  Google Scholar 

  26. Ko, W. et al. Tip-induced local strain on MoS2/graphite detected by inelastic electron tunneling spectroscopy. Phys. Rev. B 97, 125401 (2018).

    Article  CAS  Google Scholar 

  27. Marion, I. D. et al. Atomic-scale defects and electronic properties of a transferred synthesized MoS2 monolayer. Nanotechnology 29, 305703 (2018).

    Article  Google Scholar 

  28. Hong, J. et al. Exploring atomic defects in molybdenum disulphide monolayers. Nat. Commun. 6, 6293 (2015).

    Article  CAS  Google Scholar 

  29. Huang, J. L., Sung, Y. E. & Lieber, C. M. Field‐induced surface modification on the atomic scale by scanning tunneling microscopy. Appl. Phys. Lett. 61, 1528–1530 (1992).

    Article  CAS  Google Scholar 

  30. Miralrio, A., Cortes, E. R. & Castro, M. Electronic properties and enhanced reactivity of MoS2 monolayers with substitutional gold atoms embedded into sulfur vacancies. Appl. Surf. Sci. 455, 758–770 (2018).

    Article  CAS  Google Scholar 

  31. Lin, Y. C. et al. Properties of individual dopant atoms in single‐layer MoS2: atomic structure, migration, and enhanced reactivity. Adv. Mater. 26, 2857–2861 (2014).

    Article  CAS  Google Scholar 

  32. Ko, W., Ma, C., Nguyen, G. D., Kolmer, M. & Li, A. P. Atomic‐scale manipulation and in situ characterization with scanning tunneling microscopy. Adv. Funct. Mater. 29, 1903770 (2019).

    Article  CAS  Google Scholar 

  33. Scheer, E. et al. The signature of chemical valence in the electrical conduction through a single-atom contact. Nature 394, 154–157 (1998).

    Article  CAS  Google Scholar 

  34. Kresse, G. & Furthmüller, J. Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set. Comput. Mater. Sci. 6, 15–50 (1996).

    Article  CAS  Google Scholar 

  35. Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).

    Article  CAS  Google Scholar 

  36. Tersoff, J. & Hamann, D. R. Theory of the scanning tunneling microscope. Phys. Rev. B 31, 805–813 (1985).

    Article  CAS  Google Scholar 

  37. Kohn, W. & Sham, L. J. Self-consistent equations including exchange and correlation effects. Phys. Rev. 140, A1133–A1138 (1965).

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported in part by the Presidential Early Career Award for Scientists and Engineers (PECASE) through the Army Research Office (W911NF-16-1-0277), and a National Science Foundation grant (ECCS-1809017). S.M.H. acknowledges support from a US S&T Cooperation Program. The facilities of the Center for Dynamics and Control of Materials: an NSF Materials Research Science and Engineering Center (MRSEC) was used for materials characterization. A portion of this research, including STM, transport measurements and STM simulations, was conducted at the Center for Nanophase Materials Sciences at Oak Ridge National Laboratory, which is a US Department of Energy User Facility. We thank W. R. Hendren and R. M. Bowman for their help with the metal film deposition.

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Authors and Affiliations

Authors

Contributions

S.M.H. conducted the STM and transport measurements with the help of W.K. R.G. carried out the Raman spectroscopy and PL measurements. G.E.D. and F.H. prepared the large-scale exfoliated monolayer MoS2 samples. P.-A.C. and L.L. performed the atomistic simulations. S.M.H. and D.A. initiated the research on the atomistic origins of non-volatile resistance switching in single-layer atomic sheets. M.-H.C., A.-P.L. and D.A. coordinated and supervised the research. All authors contributed to the article based on the draft written by S.M.H. and D.A.

Corresponding author

Correspondence to Deji Akinwande.

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The authors declare no competing interests.

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Peer review information Nature Nanotechnology thanks Hyeon-Jin Shin 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. 1–9.

Source data

Source Data Fig. 1

Data for Fig. 1c,d.

Source Data Fig. 2

Data for Fig. 2c–f.

Source Data Fig. 3

Data for Fig. 3b,d,f.

Source Data Fig. 4

Data for Fig. 4a–d.

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Hus, S.M., Ge, R., Chen, PA. et al. Observation of single-defect memristor in an MoS2 atomic sheet. Nat. Nanotechnol. 16, 58–62 (2021). https://doi.org/10.1038/s41565-020-00789-w

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