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Deciphering the ultra-high plasticity in metal monochalcogenides

Nature Materials volume 23, pages 196–204 (2024)Cite this article

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Abstract

The quest for electronic devices that offer flexibility, wearability, durability and high performance has spotlighted two-dimensional (2D) van der Waals materials as potential next-generation semiconductors. Especially noteworthy is indium selenide, which has demonstrated surprising ultra-high plasticity. To deepen our understanding of this unusual plasticity in 2D van der Waals materials and to explore inorganic plastic semiconductors, we have conducted in-depth experimental and theoretical investigations on metal monochalcogenides (MX) and transition metal dichalcogenides (MX2). We have discovered a general plastic deformation mode in MX, which is facilitated by the synergetic effect of phase transitions, interlayer gliding and micro-cracks. This is in contrast to crystals with strong atomic bonding, such as metals and ceramics, where plasticity is primarily driven by dislocations, twinning or grain boundaries. The enhancement of gliding barriers prevents macroscopic fractures through a pinning effect after changes in stacking order. The discovery of ultra-high plasticity and the phase transition mechanism in 2D MX materials holds significant potential for the design and development of high-performance inorganic plastic semiconductors.

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Fig. 1: Atomic structures of various InSe phases (top and cross-section views) and writing capability as a pen.
Fig. 2: The structural evolution of 2H-InSe after mechanical deformation.
Fig. 3: Atomic structures near micro-cracks.
Fig. 4: In situ TEM experiments of InSe.
Fig. 5: Theoretical calculations.
Fig. 6: Schematics of the plastic deformation of MX materials.

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All data in this article 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 by the National Natural Science Foundation of China (grant nos. 52173230, 52222218 and 52272045), the Research Grants Council of Hong Kong (grant no. AoE/P-701/20), the Hong Kong Research Grant Council General Research Fund (project nos. 15301623, 11312022, 15302522, 11300820 and 15302419), the City University of Hong Kong (project nos. 6000758, 9211308, 9667223 and 9678303), The Hong Kong Polytechnic University (project nos. 1-BE47, ZE0C and ZE2F), the Environment and Conservation Fund (project nos. 69/2021 and 34/2022), the Shenzhen Science, Technology and Innovation Commission (project no. JCYJ20200109110213442), The State Key Laboratory of Marine Pollution (SKLMP) Seed Collaborative Research Fund (grant no. SKLMP/SCRF/0037) and The Research Institute for Advanced Manufacturing of The Hong Kong Polytechnic University.

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Author notes

  1. These authors contributed equally: Lok Wing Wong, Ke Yang.

Authors and Affiliations

  1. Department of Applied Physics, The Hong Kong Polytechnic University, Kowloon, Hong Kong, China

    Lok Wing Wong, Ke Yang, Wei Han, Xiaodong Zheng, Hok Yin Wong, Chi Shing Tsang, Shu Ping Lau, Ming Yang & Jiong Zhao

  2. The Hong Kong Polytechnic University Shenzhen Research Institute, Shenzhen, China

    Lok Wing Wong, Ke Yang, Wei Han, Xiaodong Zheng, Hok Yin Wong, Chi Shing Tsang, Ming Yang & Jiong Zhao

  3. Department of Chemistry and Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Kowloon, Hong Kong, China

    Chun-Sing Lee & Thuc Hue Ly

  4. Department of Chemistry and State Key Laboratory of Marine Pollution, City University of Hong Kong, Kowloon, Hong Kong, China

    Thuc Hue Ly

  5. City University of Hong Kong Shenzhen Research Institute, Shenzhen, China

    Thuc Hue Ly

  6. The Research Institute for Advanced Manufacturing, The Hong Kong Polytechnic University, Kowloon, Hong Kong, China

    Jiong Zhao

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Contributions

J.Z., M.Y. and T.H.L. led and supervised this project. L.W.W. planned the project, wrote the original manuscript and conducted focused ion beam, STEM–HAADF, in situ TEM, molecular dynamics simulations and STEM simulations. H.Y.W., X.Z., C.-S.L., S.P.L., T.H.L. and J.Z. helped data analysis. L.W.W. and W.H. prepared the materials. L.W.W., W.H. and H.Y.W. contributed to the XRD. L.W.W., W.H. and C.S.T. collected Raman data. K.Y. and M.Y. calculated the DFT results. All authors read and approved the paper.

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Correspondence to Thuc Hue Ly, Ming Yang or Jiong Zhao.

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Extended data

Extended Data Fig. 1 Raman spectra with corresponding optical images and a table of normalized peak intensity (%).

The orange crosses in the optical images indicate the laser excited position. The postdeformed InSe presents stronger E′(1) and weaker E″(2), representing 3R stacking. Exp. 4 displays a red shift with an extra peak at 199 cm−1 that attributes to some local 2R phase.

Source data

Extended Data Fig. 2 Low magnification TEM top views with selected area diffraction patterns (SAED).

a, Pristine InSe. b, Post-deformation InSe. Red circles show the selected area. Yellow circles in (a) highlight the stronger diffraction signal of {\(1\bar{2}10\)} of the pristine 2H-InSe. Scale bars: 2 µm (left), 10 1/nm (right).

Extended Data Fig. 3 Low magnification TEM cross-section views with SAED.

a, Pristine InSe. b, Post-deformation InSe. Red circles show the corresponding selected area. The average interlayer spacing is slightly shorter after deformation. Scale bars: 2 µm (left), 10 1/nm (right).

Extended Data Fig. 4 Top views of typical of low magnification STEM-HAADF after deformations.

a-f, InSe (a,b), MoS2 (c,d), and MoTe2 (e,f). Scale bars: 1 µm (a,c,e) and 200 nm (b,d,f). The orange arrows denote the serious fractures. InSe prefers relaxing strain by forming discrete micro-cracks, while MoS2 and MoTe2 prefer storing strain by dislocations, hence forming serious fracture eventually.

Extended Data Fig. 5 Cross-section view of typical low magnification STEM-HAADF after deformations.

a-i, InSe (a-c), MoS2 (d-f), and MoTe2 (g-i). InSe has significantly fewer large cracks than MoS2 and MoTe2. Scale bars: 2 µm (a-i).

Extended Data Fig. 6 Atomic cross-section views of post-deformation InSe near micro-cracks.

a, Full field of view of the post-deformed InSe supported by Si substrate. b-g, Corresponding atomic resolution STEM-HAADF highlighted by yellow boxes in (a). The grey scale (almost all the viewing area) represents 3R stacking while green, yellow, and blue in (f) highlight 3R’ stacking, phase boundary, and 2H stacking, respectively. Scale bars: 1 µm (a), 5 nm (b-g).

Extended Data Fig. 7 Atomic cross-section views of the post-deformed MoS2 near micro-cracks and defects.

a, The large field of view of the experimental MoTe2. b-e, Corresponding atomic resolution STEM-HAADF highlighted by yellow boxes in a, showing well 2H stacking. All the region demonstrates 2H stacking in MoS2 after deformation. Scale bars: 0.5 µm (a), 5 nm (b-e).

Extended Data Fig. 8 Atomic cross-section views of the post-deformed MoTe2 near micro-cracks and defects.

a, The large field of view of the experimental MoTe2. b-e, Corresponding atomic resolution STEM-HAADF highlighted by yellow boxes in a, showing well 2H stacking. All the region demonstrates 2H stacking in MoTe2 after deformation. Scale bars: 0.5 µm (a), 5 nm (b-e).

Extended Data Fig. 9 Cross-section views of the typical multilayer micro-cracks.

a, InSe. b, GaSe. Scale bars: 5 nm. The stacking near the few layers micro-cracks is mainly 3R stacking. The untransformed 2H stacking is highlighted in white in (b).

Extended Data Fig. 10 Strain analysis by geometric phase analysis of completely transformed 3R region, phase boundary and edge dislocation.

Scale bars: 2 nm. The 3R region after phase transition demonstrates strain relaxation, while the phase boundary and edge dislocation regions show strain concentration.

Supplementary information

Supplementary Information

Supplementary Figs. 1–25, Tables 1–5, Notes 1–3 and references.

Supplementary Video 1

An outermost fracture during the in situ bending experiment.

Source data

Source Data Fig. 2

Source data for Fig. 2.

Source Data Fig. 5

Source data for Fig. 5.

Source Data Extended Data Fig. 1

Source data for Extended Data Fig. 1.

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Wong, L.W., Yang, K., Han, W. et al. Deciphering the ultra-high plasticity in metal monochalcogenides. Nat. Mater. 23, 196–204 (2024). https://doi.org/10.1038/s41563-023-01788-7

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