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Unusual Dynamics of Tetrahedral Liquids Caused by the Competition between Dynamic and Structural Heterogeneity

ORAL

Abstract

Tetrahedral liquids are intriguing: they don’t pack the entire space, and they form networks of a variety of structures. As a result, tetrahedral liquids often exhibit fascinating phase behaviors like water. In this talk, I will discuss our recent neutron spin echo measurements of the collective dynamics as well as molecular dynamics (MD) simulations, using a neural network forcefield (NNFF), of another prototypical AX2-type tetrahedral network liquid, ZnCl2. We observed an unusual non-monotonic temperature-dependence of the stretching exponent β as the liquid is supercooled. Further simulations revealed that this unusual dynamic behavior is due to the competition between the decrease in the diversity of tetrahedra motifs (structural heterogeneity) and the increase of glassy dynamic heterogeneity. This result may contribute to new understandings of the unusual properties of tetrahedral liquids.

Publication: [1] S.-C. Lee, Y Z*, "Unusual dynamics of tetrahedral liquids caused by the competition between dynamic and chemical heterogeneity", J. Chem. Phys. 161, 044502 (2024).<br>[2] P. Luo, Y. Zhai, J. B. Leao, M. Kofu, K. Nakajima, A. Faraone, Y Z*, "Neutron spin echo studies of the structural relaxation of liquid ZnCl2 at the structure factor primary peak and pre-peak", J. Phys. Chem. Lett. 12(1), 392 (2021)<br>[3] P. Luo, Y. Zhai, P. Falus, V. Garcia-Sakai, M. Hartl, M. Kofu, K. Nakajima, A. Faraone, Y Z*, "Q-dependent collective relaxation dynamics of glass-forming liquid Ca0.4K0.6(NO3)1.4 investigated by wide-angle neutron spin-echo", Nature Communications 13, 2092 (2022)<br>[4] S.-C. Lee, Y. Zhai, Z. Li, N. P. Walter, M. Rose, B. J. Heuser, Y Z*, "Comparative studies of the structural and transport properties of molten salt FLiNaK using machine-learned neutral network and reparametrized classical forcefields", J. Phys. Chem. B 125(37), 10562 (2021) Featured as the journal cover art of J. Phys. Chem. B

Presenters

  • Y Z

    University of Michigan

Authors

  • Y Z

    University of Michigan

  • Shao-Chun Lee

    University of Michigan