Initial Stages of Rejuvenation of Vapor-Deposited Glasses during Isothermal Annealing: Contrast Between Experiment and Simulation

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Autori principali: Tracy, Megan E., Kasting, Benjamin J., Herrero, Cecilia, Berthier, Ludovic, Richert, Ranko, Guiseppi-Elie, Anthony, Ediger, Mark D.
Natura: Preprint
Pubblicazione: 2024
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author Tracy, Megan E.
Kasting, Benjamin J.
Herrero, Cecilia
Berthier, Ludovic
Richert, Ranko
Guiseppi-Elie, Anthony
Ediger, Mark D.
author_facet Tracy, Megan E.
Kasting, Benjamin J.
Herrero, Cecilia
Berthier, Ludovic
Richert, Ranko
Guiseppi-Elie, Anthony
Ediger, Mark D.
contents Physical vapor deposition can prepare organic glasses with high kinetic stability. When heated, these glassy solids slowly transform into the supercooled liquid in a process known as rejuvenation. In this study, we anneal vapor-deposited glasses of methyl-m-toluate (MMT) for six hours at 0.98Tg to observe rejuvenation using dielectric spectroscopy. Glasses of moderate stability exhibited partial or full rejuvenation in six hours. For highly stable glasses, prepared at substrate temperatures of 0.85Tg and 0.80Tg, the six-hour annealing time is ~2% of the estimated transformation time, and no change in the onset temperature for the α relaxation process was observed, as expected. Surprisingly, for these highly stable glasses, annealing resulted in significant increases in the storage component of the dielectric susceptibility, without corresponding increases in the loss component. These changes are interpreted to indicate that short-term annealing rejuvenates a high frequency relaxation (e.g., the boson peak) within the stable glass. We compare these results to computer simulations of the rejuvenation of highly stable glasses generated by the swap Monte Carlo algorithm. The in silico glasses, in contrast to the experiment, show no evidence of rejuvenation within the stable glass at times shorter than the alpha relaxation process.
format Preprint
id arxiv_https___arxiv_org_abs_2411_17540
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Initial Stages of Rejuvenation of Vapor-Deposited Glasses during Isothermal Annealing: Contrast Between Experiment and Simulation
Tracy, Megan E.
Kasting, Benjamin J.
Herrero, Cecilia
Berthier, Ludovic
Richert, Ranko
Guiseppi-Elie, Anthony
Ediger, Mark D.
Soft Condensed Matter
Disordered Systems and Neural Networks
Materials Science
Physical vapor deposition can prepare organic glasses with high kinetic stability. When heated, these glassy solids slowly transform into the supercooled liquid in a process known as rejuvenation. In this study, we anneal vapor-deposited glasses of methyl-m-toluate (MMT) for six hours at 0.98Tg to observe rejuvenation using dielectric spectroscopy. Glasses of moderate stability exhibited partial or full rejuvenation in six hours. For highly stable glasses, prepared at substrate temperatures of 0.85Tg and 0.80Tg, the six-hour annealing time is ~2% of the estimated transformation time, and no change in the onset temperature for the α relaxation process was observed, as expected. Surprisingly, for these highly stable glasses, annealing resulted in significant increases in the storage component of the dielectric susceptibility, without corresponding increases in the loss component. These changes are interpreted to indicate that short-term annealing rejuvenates a high frequency relaxation (e.g., the boson peak) within the stable glass. We compare these results to computer simulations of the rejuvenation of highly stable glasses generated by the swap Monte Carlo algorithm. The in silico glasses, in contrast to the experiment, show no evidence of rejuvenation within the stable glass at times shorter than the alpha relaxation process.
title Initial Stages of Rejuvenation of Vapor-Deposited Glasses during Isothermal Annealing: Contrast Between Experiment and Simulation
topic Soft Condensed Matter
Disordered Systems and Neural Networks
Materials Science
url https://arxiv.org/abs/2411.17540