Mixed equilibrium/nonequilibrium effects govern surface mobility in polymer glasses

Fuente: arXiv
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Autori principali: Xu, Jianquan, Ghanekarade, Asieh, Li, Li, Zhu, Huifeng, Yuan, Hailin, Yan, Jinsong, Simmons, David S., Tsui, Ophelia K. C., Wang, Xinping
Natura: Preprint
Pubblicazione: 2024
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author Xu, Jianquan
Ghanekarade, Asieh
Li, Li
Zhu, Huifeng
Yuan, Hailin
Yan, Jinsong
Simmons, David S.
Tsui, Ophelia K. C.
Wang, Xinping
author_facet Xu, Jianquan
Ghanekarade, Asieh
Li, Li
Zhu, Huifeng
Yuan, Hailin
Yan, Jinsong
Simmons, David S.
Tsui, Ophelia K. C.
Wang, Xinping
contents The temperature at which supercooled liquids turn into solid-like glasses ($T_g$) can change at the free surface, affecting the properties of nanostructured glasses and their applications. However, inadequate experimental resolution to determine the $T_g$ gradient and a longstanding debate over the role of nonequilibrium effects have hindered fundamental understanding of this phenomenon. Using spatially resolved $T_g$ measurements and molecular dynamics simulations, we reveal a crossover from equilibrium behavior to a new regime of near-surface nonequilibrium glass physics on cooling. This crossover causes the form of the nonequilibrium $T_g$ gradient to change, highlighting the need to include these physics for rational understanding of the properties of realistic nanostructured glass-forming materials. They also potentially recast the interpretation of decades of experimental data on nanoconfined glasses.
format Preprint
id arxiv_https___arxiv_org_abs_2402_06917
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Mixed equilibrium/nonequilibrium effects govern surface mobility in polymer glasses
Xu, Jianquan
Ghanekarade, Asieh
Li, Li
Zhu, Huifeng
Yuan, Hailin
Yan, Jinsong
Simmons, David S.
Tsui, Ophelia K. C.
Wang, Xinping
Soft Condensed Matter
Materials Science
The temperature at which supercooled liquids turn into solid-like glasses ($T_g$) can change at the free surface, affecting the properties of nanostructured glasses and their applications. However, inadequate experimental resolution to determine the $T_g$ gradient and a longstanding debate over the role of nonequilibrium effects have hindered fundamental understanding of this phenomenon. Using spatially resolved $T_g$ measurements and molecular dynamics simulations, we reveal a crossover from equilibrium behavior to a new regime of near-surface nonequilibrium glass physics on cooling. This crossover causes the form of the nonequilibrium $T_g$ gradient to change, highlighting the need to include these physics for rational understanding of the properties of realistic nanostructured glass-forming materials. They also potentially recast the interpretation of decades of experimental data on nanoconfined glasses.
title Mixed equilibrium/nonequilibrium effects govern surface mobility in polymer glasses
topic Soft Condensed Matter
Materials Science
url https://arxiv.org/abs/2402.06917