Many-Body Correlations Are Non-negligible in Both Fragile and Strong Glassformers.
Phys Rev Lett
; 129(14): 145501, 2022 Sep 30.
Article
em En
| MEDLINE
| ID: mdl-36240416
ABSTRACT
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.
Texto completo:
1
Bases de dados:
MEDLINE
Idioma:
En
Revista:
Phys Rev Lett
Ano de publicação:
2022
Tipo de documento:
Article
País de afiliação:
Holanda