Generalized mode-coupling theory of the glass transition. I. Numerical results for Percus–Yevick hard spheres

Mode-coupling theory (MCT) constitutes one of the few first-principles-based approaches to describe the physics of the glass transition, but the theory’s inherent approximations compromise its accuracy in the activated glassy regime. Here, we show that microscopic generalized mode-coupling theory (GMCT), a recently proposed hierarchical framework to systematically improve upon MCT, provides a promising pathway toward a more accurate first-principles description of glassy dynamics. We present a comprehensive numerical analysis for Percus–Yevick hard spheres by performing explicitly wavenumber- and time-dependent GMCT calculations up to sixth order. Specifically, we calculate the location of the critical point, the associated non-ergodicity parameters, and the time-dependent dynamics of the density correlators at both absolute and reduced packing fractions, and we test several universal scaling relations in the α- and β-relaxation regimes. It is found that higher-order GMCT can successfully remedy some of MCT’s pathologies, including an underestimation of the critical glass transition density and an overestimation of the hard-sphere fragility. Furthermore, we numerically demonstrate that the celebrated scaling laws of MCT are preserved in GMCT and that the predicted critical exponents manifestly improve as more levels are incorporated in the GMCT hierarchy. Although formally the GMCT equations should be solved up to infinite order to reach full convergence, our finite-order GMCT calculations unambiguously reveal a uniform convergence pattern for the dynamics. We thus argue that GMCT can provide a feasible and controlled means to bypass MCT’s main uncontrolled approximation, offering hope for the future development of a quantitative first-principles theory of the glass transition.