Ref HAL: hal-03662093_v1
Ref Arxiv: 2103.01569
DOI: 10.1038/s41567-022-01508-z
WoS: WOS:000770232200001
Ref. & Cit.: NASA ADS
Exporter : BibTex | endNote
Résumé:

Glass formation is encountered in diverse materials. Experiments have revealed that dynamic relaxation spectra of supercooled liquids generically become asymmetric near the glass transition temperature, Tg, where an extended power law emerges at high frequencies. The microscopic origin of this "wing" remains unknown, and was so far inaccessible to simulations. Here, we develop a novel computational approach and study the equilibrium dynamics of model supercooled liquids near Tg. We demonstrate the emergence of a power law wing in numerical spectra, which originates from relaxation at rare, localised regions over broadly-distributed timescales. We rationalise the asymmetric shape of relaxation spectra by constructing an empirical model associating heterogeneous activated dynamics with dynamic facilitation, which are the two minimal physical ingredients revealed by our simulations. Our work offers a glimpse of the molecular motion responsible for glass formation at relevant experimental conditions.