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Ion diffusion retarded by diverging chemical susceptibility

Author

Listed:
  • Yuhang Cai

    (Berkeley
    Lawrence Berkeley National Laboratory)

  • Zhaowu Wang

    (Hebei University of Technology
    Nanjing University)

  • Jiawei Wan

    (Berkeley
    Lawrence Berkeley National Laboratory)

  • Jiachen Li

    (Berkeley
    Lawrence Berkeley National Laboratory)

  • Ruihan Guo

    (Berkeley
    Lawrence Berkeley National Laboratory)

  • Joel W. Ager

    (Berkeley
    Lawrence Berkeley National Laboratory)

  • Ali Javey

    (Lawrence Berkeley National Laboratory
    Berkeley)

  • Haimei Zheng

    (Berkeley
    Lawrence Berkeley National Laboratory)

  • Jun Jiang

    (University of Science and Technology of China)

  • Junqiao Wu

    (Berkeley
    Lawrence Berkeley National Laboratory)

Abstract

For first-order phase transitions, the second derivatives of Gibbs free energy (specific heat and compressibility) diverge at the transition point, resulting in an effect known as super-elasticity along the pressure axis, or super-thermicity along the temperature axis. Here we report a chemical analogy of these singularity effects along the atomic doping axis, where the second derivative of Gibbs free energy (chemical susceptibility) diverges at the transition point, leading to an anomalously high energy barrier for dopant diffusion in co-existing phases, an effect we coin as super-susceptibility. The effect is realized in hydrogen diffusion in vanadium dioxide (VO2) with a metal-insulator transition (MIT). We show that hydrogen faces three times higher energy barrier and over one order of magnitude lower diffusivity when it diffuses across a metal-insulator domain wall in VO2. The additional energy barrier is attributed to a volumetric energy penalty that the diffusers need to pay for the reduction of latent heat. The super-susceptibility and resultant retarded atomic diffusion are expected to exist universally in all phase transformations where the transformation temperature is coupled to chemical composition, and inspires new ways to engineer dopant diffusion in phase-coexisting material systems.

Suggested Citation

  • Yuhang Cai & Zhaowu Wang & Jiawei Wan & Jiachen Li & Ruihan Guo & Joel W. Ager & Ali Javey & Haimei Zheng & Jun Jiang & Junqiao Wu, 2024. "Ion diffusion retarded by diverging chemical susceptibility," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-50213-3
    DOI: 10.1038/s41467-024-50213-3
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    References listed on IDEAS

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    1. Yuliang Chen & Zhaowu Wang & Shi Chen & Hui Ren & Liangxin Wang & Guobin Zhang & Yalin Lu & Jun Jiang & Chongwen Zou & Yi Luo, 2018. "Non-catalytic hydrogenation of VO2 in acid solution," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    2. Jian Shi & You Zhou & Shriram Ramanathan, 2014. "Colossal resistance switching and band gap modulation in a perovskite nickelate by electron doping," Nature Communications, Nature, vol. 5(1), pages 1-9, December.
    3. Jikun Chen & Wei Mao & Binghui Ge & Jiaou Wang & Xinyou Ke & Vei Wang & Yiping Wang & Max Döbeli & Wentong Geng & Hiroyuki Matsuzaki & Jian Shi & Yong Jiang, 2019. "Revealing the role of lattice distortions in the hydrogen-induced metal-insulator transition of SmNiO3," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    4. Jae Hyung Park & Jim M. Coy & T. Serkan Kasirga & Chunming Huang & Zaiyao Fei & Scott Hunter & David H. Cobden, 2013. "Measurement of a solid-state triple point at the metal–insulator transition in VO2," Nature, Nature, vol. 500(7463), pages 431-434, August.
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