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Non-Gaussian energy landscape of a simple model for strong network-forming liquids: accurate evaluation of the configurational entropy

A. J. Moreno·I. Saika-Voivod·E. Zaccarelli·E. La Nave·S. V. Buldyrev·P. Tartaglia·F. Sciortino
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Abstract

We present a numerical study of the statistical properties of the potential energy landscape of a simple model for strong network-forming liquids. The model is a system of spherical particles interacting through a square well potential, with an additional constraint that limits the maximum number of bonds, $N_{\rm max}$, per particle. Extensive simulations have been carried out as a function of temperature, packing fraction, and $N_{\rm max}$. The dynamics of this model are characterized by Arrhenius temperature dependence of the transport coefficients and by nearly exponential relaxation of dynamic correlators, i.e. features defining strong glass-forming liquids. This model has two important features: (i) landscape basins can be associated with bonding patterns; (ii) the configurational volume of the basin can be evaluated in a formally exact way, and numerically with arbitrary precision. These features allow us to evaluate the number of different topologies the bonding pattern can adopt. We find that the number of fully bonded configurations, i.e. configurations in which all particles are bonded to $N_{\rm max}$ neighbors, is extensive, suggesting that the configurational entropy of the low temperature fluid is finite. We also evaluate the energy dependence of the configurational entropy close to the fully bonded state, and show that it follows a logarithmic functional form, differently from the quadratic dependence characterizing fragile liquids. We suggest that the presence of a discrete energy scale, provided by the particle bonds, and the intrinsic degeneracy of fully bonded disordered networks differentiates strong from fragile behavior.

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A. J. Moreno, I. Saika-Voivod, E. Zaccarelli, E. La Nave, S. V. Buldyrev, P. Tartaglia, F. Sciortino. 2006-05-29. Non-Gaussian energy landscape of a simple model for strong network-forming liquids: accurate evaluation of the configurational entropy. https://doi.org/10.1063/1.2196879

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