Many-Body Correlations are Non-negligible in Both Fragile and Strong Glassformers
CJ Luo and JF Robinson and I Pihlajamaa and VE Debets and CP Royall and LMC Janssen, PHYSICAL REVIEW LETTERS, 129, 145501 (2022).
It is widely believed that the emergence of slow glassy dynamics is encoded in a material's microstructure. First-principles theory mode- coupling theory (MCT) is able to predict the dramatic slowdown of the dynamics from only static two-point correlations as input, yet it cannot capture all of the observed dynamical behavior. Here we go beyond two- point spatial correlation functions by extending MCT systematically to include higher-order static and dynamic correlations. We demonstrate that only adding the static triplet direct correlations already qualitatively changes the predicted glass-transition diagram of binary hard spheres and silica. Moreover, we find a nontrivial competition between static triplet correlations that work to stabilize the glass state and dynamic higher-order correlations that destabilize it for both materials. We conclude that the conventionally neglected static triplet direct correlations as well as higher-order dynamic correlations are, in fact, non-negligible in both fragile and strong glassformers.
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