TY - JOUR

T1 - On a fundamental description of the Kovacs’ kinetic signatures in glass-forming systems

AU - Lira-Escobedo, J.

AU - Mendoza-Méndez, P.

AU - Medina-Noyola, M.

AU - McKenna, G. B.

AU - Ramírez-González, P. E.

N1 - Funding Information:
The authors appreciate the technical assistance of J. Limón Castillo. They acknowledge the financial support of CONACyT through Cátedras CONACyT Grant No. 1631 and CB-2015-01 Grant No. 257636. The authors would like to thank LANIMFE for the infrastructure provided during this project. G.B.M. would like to acknowledge the partial support from the J. R. Bradford Endowment at Texas Tech University and the U.S. National Science Foundation, under Grant No. DMR-207070.
Publisher Copyright:
© 2021 Author(s).

PY - 2021/7/7

Y1 - 2021/7/7

N2 - The time-evolution equation for the time-dependent static structure factor of the non-equilibrium self-consistent generalized Langevin equation (NE-SCGLE) theory was used to investigate the kinetics of glass-forming systems under isochoric conditions. The kinetics are studied within the framework of the fictive temperature (TF) of the glassy structure. We solve for the kinetics of TF(t) and the time-dependent structure factor and find that they are different but closely related by a function that depends only on temperature. Furthermore, we are able to solve for the evolution of TF(t) in a set of temperature-jump histories referred to as the Kovacs’ signatures. We demonstrate that the NE-SCGLE theory reproduces all the Kovacs’ signatures, namely, intrinsic isotherm, asymmetry of approach, and memory effect. In addition, we extend the theory into largely unexplored, deep glassy state, regions that are below the notionally “ideal” glass temperature.

AB - The time-evolution equation for the time-dependent static structure factor of the non-equilibrium self-consistent generalized Langevin equation (NE-SCGLE) theory was used to investigate the kinetics of glass-forming systems under isochoric conditions. The kinetics are studied within the framework of the fictive temperature (TF) of the glassy structure. We solve for the kinetics of TF(t) and the time-dependent structure factor and find that they are different but closely related by a function that depends only on temperature. Furthermore, we are able to solve for the evolution of TF(t) in a set of temperature-jump histories referred to as the Kovacs’ signatures. We demonstrate that the NE-SCGLE theory reproduces all the Kovacs’ signatures, namely, intrinsic isotherm, asymmetry of approach, and memory effect. In addition, we extend the theory into largely unexplored, deep glassy state, regions that are below the notionally “ideal” glass temperature.

UR - http://www.scopus.com/inward/record.url?scp=85109007404&partnerID=8YFLogxK

U2 - 10.1063/5.0054520

DO - 10.1063/5.0054520

M3 - Article

C2 - 34241391

AN - SCOPUS:85109007404

VL - 155

JO - The Journal of Chemical Physics

JF - The Journal of Chemical Physics

SN - 0021-9606

IS - 1

M1 - 014503

ER -