Vapor-deposited alcohol glasses reveal a wide range of kinetic stability

Tylinski, M.; Chua, Yeong Zen; Beasley, M. S.; Schick, Christoph; Ediger, M. D.

doi:10.1063/1.4966582

Cited by 39 publications

(53 citation statements)

References 112 publications

(278 reference statements)

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“…f BA T gðBAÞ and the T g(BA) = 168 K, 68 with T g(LA) = 50 1C and f BA = 0.05, one recovers an average T g(LA/BA) value of around 35 1C. This value is not far from room temperature especially taking into account the large polymer polydispersity leading probably to mobile parts at room temperature.…”

Section: Heterogeneous Water Invasion (Formation Of Cavities)mentioning

confidence: 62%

Swelling, dewetting and breakup in thin polymer films for cultural heritage

et al. 2020

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Section: Heterogeneous Water Invasion (Formation Of Cavities)mentioning

confidence: 62%

Swelling, dewetting and breakup in thin polymer films for cultural heritage

et al. 2020

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“…Predicting and controlling the properties of PVD glasses formed with different types of small organic molecules remains a fundamental challenge. In particular, intermolecular interactions seem to have a large effect on the stability of PVD films [28][29][30][31]. This was demonstrated recently by Laventure et.…”

Section: Introductionmentioning

confidence: 93%

Effects of microstructure formation on the stability of vapor-deposited glasses

Moore

Huang

Wolf

et al. 2019

Proc. Natl. Acad. Sci. U.S.A.

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Glasses formed by physical vapor deposition (PVD) are an interesting new class of materials, exhibiting properties thought to be equivalent to those of glasses aged for thousands of years. Exerting control over the structure and properties of PVD glasses formed with different types of glass-forming molecules is now an emerging challenge. In this work, we study coarse grained models of organic glass formers containing fluorocarbon tails of increasing length, corresponding to an increased tendency to form microstructures. We use simulated PVD to examine how the presence of the microphase separated domains in the supercooled liquid influences the ability to form stable glasses. This model suggests that increasing molecule tail length results in decreased thermodynamic and kinetic stability of the molecules in PVD films. The reduced stability is further linked to the reduced ability of these molecules to equilibrate at the free surface during PVD. We find that as the tail length is increased, the relaxation time near the surface of the supercooled equilibrium liquid films of these molecules are slowed and become essentially bulk-like, due to the segregation of the fluorocarbon tails to the free surface. Surface diffusion is also markedly reduced due to clustering of the molecules at the surface. Based on these results, we propose a trapping mechanism where tails are unable to move between local phase separated domains on the relevant deposition time scales.

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“…However, the typical time it takes to the system to converge to this long-t w plateau, depends drastically on the final temperature. This is more clearly seen by plotting ∆(t + t w , t w )/T for t = 2 22 [i.e. the long t limit of the mean-squared displacement (MSD)] as function of t w , see Fig.…”

Section: B Growing Timescales Upon Coolingmentioning

confidence: 98%

“…Compared to their liquid-cooled counterparts, vapor-deposited glasses show higher density [16] and kinetic stability [15,17]. When these ultra-stable glasses are studied at very low temperatures, it is found that the anomalies characteristic of amorphous solids are strongly supressed [18][19][20][21][22].Many theoretical approaches to this problem are based on the study of the potential energy landscape of glassforming particle systems [13,[23][24][25][26][27][28]. These studies have suggested that glass anomalies can be interpreted in terms of glass states being not well-defined energy minima, but structured metabasins containing a collection of sub-basins separated by barriers of variable size [29,30], see Fig.…”

mentioning

confidence: 99%

Low-temperature anomalies of a vapor deposited glass

Seoane

Reid

Pablo

et al. 2018

Phys. Rev. Materials

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We investigate the low temperature properties of two-dimensional Lennard-Jones glass films, prepared in silico both by liquid cooling and by physical vapor deposition. We identify deep in the solid phase a crossover temperature T * , at which slow dynamics and enhanced heterogeneity emerge. Around T * , localized defects become visible, leading to vibrational anomalies as compared to standard solids. We find that on average, T * decreases in samples with lower inherent structure energy, suggesting that such anomalies will be suppressed in ultra-stable glass films, prepared both by very slow liquid cooling and vapor deposition.Low-temperature crystalline solids are usually described in terms of harmonic vibrations around a perfect periodic lattice (phonons). Within this framework, defects such as vacancies and dislocations can be treated as small perturbations. This description breaks down for amorphous solids such as glasses, foams, emulsions, plastics, colloids, granular materials, bacterial colonies, and tissues [1][2][3][4][5][6][7]. In these systems, the identification of "defects" becomes challenging because the solid ground state is strongly disordered. As a consequence, amorphous solids display many universal anomalies with respect to crystals. Examples are the so-called Boson Peak, an excess of low-energy vibrational modes [8]; the anomalous scaling of heat capacity and thermal conductivity with temperature [9,10]; the irreversible plastic response to arbitrarily small perturbations [1,3,4,11]; and highly cooperative relaxation dynamics, contributing to the socalled β-processes [12][13][14].These anomalies have been widely reported in amorphous solids of very different nature. Interestingly, recent experimental work has shown that by preparing glasses through a process of physical vapor deposition, one can produce ultra-stable states that lie deep in the free energy landscape [15]. Compared to their liquid-cooled counterparts, vapor-deposited glasses show higher density [16] and kinetic stability [15,17]. When these ultra-stable glasses are studied at very low temperatures, it is found that the anomalies characteristic of amorphous solids are strongly supressed [18][19][20][21][22].Many theoretical approaches to this problem are based on the study of the potential energy landscape of glassforming particle systems [13,[23][24][25][26][27][28]. These studies have suggested that glass anomalies can be interpreted in terms of glass states being not well-defined energy minima, but structured metabasins containing a collection of sub-basins separated by barriers of variable size [29,30], see Fig. 1. In particular, recent work [31][32][33] has identified a set of simple observables (the mean square displacement between identical "clones" of the original system) that allows one to detect easily the development of a structure of sub-basins inside a glass metabasin.In this work, using the methods of [31-33], we explore in silico the potential energy landscape of binary Lennard-Jones glass films prepared through tw...

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Vapor-deposited alcohol glasses reveal a wide range of kinetic stability

Cited by 39 publications

References 112 publications

Swelling, dewetting and breakup in thin polymer films for cultural heritage

Swelling, dewetting and breakup in thin polymer films for cultural heritage

Effects of microstructure formation on the stability of vapor-deposited glasses

Low-temperature anomalies of a vapor deposited glass

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