The nonlinear physical aging-susceptibility of a glass forming melt

Abstract

A high-resolution, temperature oscillation-based probe of physical aging in complex systems is introduced. The Fourier analysis of the measured responses allows one to extract a high-order aging-related complex susceptibility that is not accessible via traditional temperature-jump and -ramp procedures. To demonstrate the potential of this oscillatory approach, we analyze the periodic time evolution of glycerol's structural relaxation using shear rheology as a vehicle. Thereby, we access up to the sixth harmonics and detect aging fingerprints within a resolution range of three orders of magnitude for temperature amplitudes of up to 4 K. The high-order aging coefficients and susceptibilities obtained for glycerol are described well by the Tool-Narayanaswami-Moynihan formalism.