Abstract
The emergence of glassy dynamics and the glass transition in dense disordered systems is still not fully understood theoretically. Mode-coupling theory (MCT) has shown to be effective in describing some of the non-trivial features of glass formation, but it cannot explain the full glassy phenomenology due to the strong approximations on which it is based. Generalized mode-coupling theory (GMCT) is a hierarchical extension of the theory, which is able to outclass MCT by carefully describing the dynamics of higher-order correlations in its generalized framework. Unfortunately, the theory has so far only been developed for single-component systems and as a result works poorly for highly polydisperse materials. In this paper, we solve this problem by developing GMCT for multi-component systems. We use it to predict the glassy dynamics of the binary Kob–Andersen Lennard-Jones mixture, as well as its purely repulsive Weeks–Chandler–Andersen analogue. Our results show that each additional level of the GMCT hierarchy gradually improves the predictive power of GMCT beyond its previous limit. This implies that our theory is able to harvest more information from the static correlations, thus being able to better understand the role of attraction in supercooled liquids from a first-principles perspective.Graphic abstract
Highlights
Understanding how supercooled liquids become rigid and turn into amorphous solids is still one of the major challenges in condensed matter physics [1–4]
The strength of Generalized mode-coupling theory (GMCT) is its capability of predicting dynamics from statics
The first result that we show underlines the sensitivity of GMCT to small variations in the static structure
Summary
Understanding how supercooled liquids become rigid and turn into amorphous solids is still one of the major challenges in condensed matter physics [1–4] This socalled glass transition is not a transition in the thermodynamic sense [5], but it is defined by the dramatic increase in viscosity (or relaxation time) upon only a relatively slight change in thermodynamic control parameters, e.g., temperature or density [6,7]. Promising methodical MCT correction efforts have been put forward for single-component systems— or equivalently systems with a small degree of polydispersity—using higher-order field-theoretic loop expansions [27–32]. Results show that such an expansion can be accomplished, producing a novel, hierarchical first-principles theory known as generalized MCT (GMCT). By systematically developing the hierarchical equations, GMCT has already proven to be capable of predicting the microscopic dynamics of glassy mate-
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