Microscopic relation between fictive temperature and fragility from configurational enthalpy fluctuations

The fragility parameter m and the fictive temperature Tf(t) are central quantities in the description of glass formation and structural arrest. Calorimetric studies have long established a connection between fragility, cooling rate, and the frozen fictive temperature. Here, we develop a microscopic dynamical basis for this connection by relating Tf(t) to configurational enthalpy fluctuations. The delayed configurational enthalpy response is governed by the normalized enthalpy-enthalpy time-correlation function, which also determines the configurational part of the frequency-dependent heat capacity. The fictive temperature follows from this delayed enthalpy response, while fragility enters separately through the temperature dependence of the structural relaxation time and hence through the material-time clock. This separation leads to a general memory expression for the full time-dependent Tf(t), with the familiar Tool equation emerging in the Debye limit. The formulation, therefore, distinguishes two roles: the enthalpy correlation function determines the relaxation kernel, whereas fragility determines how rapidly that kernel is traversed during cooling. The conventional cooling-rate dependence of the frozen fictive temperature then appears as a limiting consequence rather than the starting point of the theory. Quantitative prediction deep in the nonequilibrium glass requires a continuation of the structural clock to depend on both T and Tf.

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Publication Details

Journal
The Journal of Chemical Physics
Published
2026-10-26
DOI
https://doi.org/10.1063/5.0344258
Primary Topic
Material Dynamics and Properties
Type
article
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article

Microscopic relation between fictive temperature and fragility from configurational enthalpy fluctuations

Biman Bagchi
The Journal of Chemical Physics
Material Dynamics and Properties
article

Microscopic relation between fictive temperature and fragility from configurational enthalpy fluctuations

Biman Bagchi
article en

Abstract

The fragility parameter m and the fictive temperature Tf(t) are central quantities in the description of glass formation and structural arrest. Calorimetric studies have long established a connection between fragility, cooling rate, and the frozen fictive temperature. Here, we develop a microscopic dynamical basis for this connection by relating Tf(t) to configurational enthalpy fluctuations. The delayed configurational enthalpy response is governed by the normalized enthalpy-enthalpy time-correlation function, which also determines the configurational part of the frequency-dependent heat capacity. The fictive temperature follows from this delayed enthalpy response, while fragility enters separately through the temperature dependence of the structural relaxation time and hence through the material-time clock. This separation leads to a general memory expression for the full time-dependent Tf(t), with the familiar Tool equation emerging in the Debye limit. The formulation, therefore, distinguishes two roles: the enthalpy correlation function determines the relaxation kernel, whereas fragility determines how rapidly that kernel is traversed during cooling. The conventional cooling-rate dependence of the frozen fictive temperature then appears as a limiting consequence rather than the starting point of the theory. Quantitative prediction deep in the nonequilibrium glass requires a continuation of the structural clock to depend on both T and Tf.

The Journal of Chemical PhysicsVol. 165(16)
Indian Institute of Science Bangalore (IN)
Openalex Percentile: Top 29%
Material Dynamics and Properties
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