Influence of Substrate Temperature on the Transformation Front Velocities That Determine Thermal Stability of Vapor-Deposited Glasses

Dalal, Shakeel S.; Ediger, M. D.

doi:10.1021/jp512905a

Title: Influence of Substrate Temperature on the Transformation Front Velocities That Determine Thermal Stability of Vapor-Deposited Glasses

Abstract

Stable organic glasses prepared by physical vapor deposition transform into the supercooled liquid via propagating fronts of molecular mobility, a mechanism different from that exhibited by glasses prepared by cooling the liquid. In this paper, we show that spectroscopic ellipsometry can directly observe this front-based mechanism in real time and explore how the velocity of the front depends upon the substrate temperature during deposition. For the model glass former indomethacin, we detect surface-initiated mobility fronts in glasses formed at substrate temperatures between 0.68T_g and 0.94T_g. At each of two annealing temperatures, the substrate temperature during deposition can change the transformation front velocity by a factor of 6, and these changes are imperfectly correlated with the density of the glass. We also observe substrate-initiated fronts at some substrate temperatures. By connecting with theoretical work, we are able to infer the relative mobilities of stable glasses prepared at different substrate temperatures. Finally, an understanding of the transformation behavior of vapor-deposited glasses may be relevant for extending the lifetime of organic semiconducting devices.

Authors:

Dalal, Shakeel S. ^[1]; Ediger, M. D. ^[1]

Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemistry

Publication Date:: Mon Feb 09 00:00:00 EST 2015

Research Org.:: Univ. of Wisconsin, Madison, WI (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1433858

Grant/Contract Number:: SC0002161

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

Additional Journal Information:: Journal Volume: 119; Journal Issue: 9; Journal ID: ISSN 1520-6106

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; organic glasses; mobility fronts; vapor-deposited glasses; growth fronts; amorphous solids; spectroscopic ellipsometry; supercooled liquids; glass transformation; stable glass

Citation Formats


                    Dalal, Shakeel S., and Ediger, M. D. Influence of Substrate Temperature on the Transformation Front Velocities That Determine Thermal Stability of Vapor-Deposited Glasses.  United States: N. p., 2015. 
Web.  doi:10.1021/jp512905a.

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                    Dalal, Shakeel S., & Ediger, M. D. Influence of Substrate Temperature on the Transformation Front Velocities That Determine Thermal Stability of Vapor-Deposited Glasses.  United States.  https://doi.org/10.1021/jp512905a

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                    Dalal, Shakeel S., and Ediger, M. D. Mon .  
"Influence of Substrate Temperature on the Transformation Front Velocities That Determine Thermal Stability of Vapor-Deposited Glasses".  United States.  https://doi.org/10.1021/jp512905a.  https://www.osti.gov/servlets/purl/1433858.

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@article{osti_1433858,

  title        = {Influence of Substrate Temperature on the Transformation Front Velocities That Determine Thermal Stability of Vapor-Deposited Glasses},

  author       = {Dalal, Shakeel S. and Ediger, M. D.},

  abstractNote = {Stable organic glasses prepared by physical vapor deposition transform into the supercooled liquid via propagating fronts of molecular mobility, a mechanism different from that exhibited by glasses prepared by cooling the liquid. In this paper, we show that spectroscopic ellipsometry can directly observe this front-based mechanism in real time and explore how the velocity of the front depends upon the substrate temperature during deposition. For the model glass former indomethacin, we detect surface-initiated mobility fronts in glasses formed at substrate temperatures between 0.68Tg and 0.94Tg. At each of two annealing temperatures, the substrate temperature during deposition can change the transformation front velocity by a factor of 6, and these changes are imperfectly correlated with the density of the glass. We also observe substrate-initiated fronts at some substrate temperatures. By connecting with theoretical work, we are able to infer the relative mobilities of stable glasses prepared at different substrate temperatures. Finally, an understanding of the transformation behavior of vapor-deposited glasses may be relevant for extending the lifetime of organic semiconducting devices.},

  doi          = {10.1021/jp512905a},

  journal      = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},

  number       = 9,

  volume       = 119,

  place        = {United States},

  year         = {Mon Feb 09 00:00:00 EST 2015},

  month        = {Mon Feb 09 00:00:00 EST 2015}

}

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Works referenced in this record:

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Fluctuating mobility generation and transport in glasses
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Evaluation of Growth Front Velocity in Ultrastable Glasses of Indomethacin over a Wide Temperature Interval
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Model vapor-deposited glasses: Growth front and composition effects
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Works referencing / citing this record:

Transformation kinetics of vapor-deposited thin film organic glasses: the role of stability and molecular packing anisotropy
journal, January 2015

Rodríguez-Tinoco, Cristian; Gonzalez-Silveira, Marta; Ràfols-Ribé, Joan
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Glass softening kinetics in the limit of high heating rates
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Cubeta, Ulyana S.; Sadtchenko, Vlad
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Surface-Bulk Interplay in Vapor-Deposited Glasses: Crossover Length and the Origin of Front Transformation
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Flenner, Elijah; Berthier, Ludovic; Charbonneau, Patrick
Physical Review Letters, Vol. 123, Issue 17
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Title: Influence of Substrate Temperature on the Transformation Front Velocities That Determine Thermal Stability of Vapor-Deposited Glasses

Abstract

Citation Formats

Relaxation in glassforming liquids and amorphous solids journal, September 2000

Organic Glasses with Exceptional Thermodynamic and Kinetic Stability journal, January 2007

Influence of substrate temperature on the stability of glasses prepared by vapor deposition journal, October 2007

Anisotropic Structure and Transformation Kinetics of Vapor-Deposited Indomethacin Glasses journal, January 2011

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Suppression of tunneling two-level systems in ultrastable glasses of indomethacin journal, July 2014

Hiking down the Energy Landscape: Progress Toward the Kauzmann Temperature via Vapor Deposition journal, April 2008

Highly Stable Vapor-Deposited Glasses of Four Tris-naphthylbenzene Isomers journal, October 2011

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Reorganization of the molecular orientation at the organic/substrate interface in spirofluorene thin films journal, March 2013

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Stable glasses of indomethacin and α,α,β-tris-naphthylbenzene transform into ordinary supercooled liquids journal, November 2012

Manipulating the properties of stable organic glasses using kinetic facilitation journal, March 2013

One Micrometer Length Scale Controls Kinetic Stability of Low-Energy Glasses journal, November 2009

Anomalous Transformation of Vapor-Deposited Highly Stable Glasses of Toluene into Mixed Glassy States by Annealing Above T g journal, March 2012

Fluctuating mobility generation and transport in glasses journal, August 2013

Evaluation of Growth Front Velocity in Ultrastable Glasses of Indomethacin over a Wide Temperature Interval journal, August 2014

Model vapor-deposited glasses: Growth front and composition effects journal, October 2013

Macroscopic facilitation of glassy relaxation kinetics: Ultrastable glass films with frontlike thermal response journal, December 2010

A Model of Structural Relaxation in Glass journal, October 1971

Structural Variations of an Organic Glassformer Vapor-Deposited onto a Temperature Gradient Stage journal, February 2011

Molecular Orientation in Stable Glasses of Indomethacin journal, April 2012

Observation of low heat capacities for vapor-deposited glasses of indomethacin as determined by AC nanocalorimetry journal, July 2010

Broadband Dielectric Relaxation Study at Ambient and Elevated Pressure of Molecular Dynamics of Pharmaceutical: Indomethacin journal, September 2009

The Temperature Dependence of Relaxation Mechanisms in Amorphous Polymers and Other Glass-forming Liquids journal, July 1955

Structural relaxation in the glass: Evidence for a path dependence of the relaxation time journal, November 2006

On the surface of glasses journal, December 2008

Surface Self-Diffusion of an Organic Glass journal, June 2011

Surface Self-Diffusion of Organic Glasses journal, August 2013

Some quantum weirdness in physiology journal, October 2009

Molecular view of the isothermal transformation of a stable glass to a liquid journal, June 2008

Equilibrium ultrastable glasses produced by random pinning journal, December 2014

Transformation kinetics of vapor-deposited thin film organic glasses: the role of stability and molecular packing anisotropy journal, January 2015

Phase separation during bulk polymerization of methyl methacrylate journal, November 2018

Perspective: Highly stable vapor-deposited glasses journal, December 2017

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Relaxation in glassforming liquids and amorphous solids
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Organic Glasses with Exceptional Thermodynamic and Kinetic Stability
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Influence of substrate temperature on the stability of glasses prepared by vapor deposition
journal, October 2007

Anisotropic Structure and Transformation Kinetics of Vapor-Deposited Indomethacin Glasses
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High-Throughput Ellipsometric Characterization of Vapor-Deposited Indomethacin Glasses
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Character of Devitrification, Viewed from Enthalpic Paths, of the Vapor-Deposited Ethylbenzene Glasses
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Highly stable glasses of celecoxib: Influence on thermo-kinetic properties, microstructure and response towards crystal growth
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Enthalpy and high temperature relaxation kinetics of stable vapor-deposited glasses of toluene
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Suppression of tunneling two-level systems in ultrastable glasses of indomethacin
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Hiking down the Energy Landscape: Progress Toward the Kauzmann Temperature via Vapor Deposition
journal, April 2008

Highly Stable Vapor-Deposited Glasses of Four Tris-naphthylbenzene Isomers
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Density and birefringence of a highly stable α,α,β-trisnaphthylbenzene glass
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Molecular orientation in small-molecule organic light-emitting diodes
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Wide-Range Refractive Index Control of Organic Semiconductor Films Toward Advanced Optical Design of Organic Optoelectronic Devices
journal, September 2012

A molecular view of vapor deposited glasses
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Real-Time Measurement of Molecular Orientational Randomization Dynamics during Annealing Treatments by In-Situ Ellipsometry
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Reorganization of the molecular orientation at the organic/substrate interface in spirofluorene thin films
journal, March 2013

Stable Glass Transformation to Supercooled Liquid via Surface-Initiated Growth Front
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Stable glasses of indomethacin and α,α,β-tris-naphthylbenzene transform into ordinary supercooled liquids
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Manipulating the properties of stable organic glasses using kinetic facilitation
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One Micrometer Length Scale Controls Kinetic Stability of Low-Energy Glasses
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Anomalous Transformation of Vapor-Deposited Highly Stable Glasses of Toluene into Mixed Glassy States by Annealing Above T _g
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Fluctuating mobility generation and transport in glasses
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Evaluation of Growth Front Velocity in Ultrastable Glasses of Indomethacin over a Wide Temperature Interval
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Model vapor-deposited glasses: Growth front and composition effects
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A Model of Structural Relaxation in Glass
journal, October 1971

Structural Variations of an Organic Glassformer Vapor-Deposited onto a Temperature Gradient Stage
journal, February 2011

Molecular Orientation in Stable Glasses of Indomethacin
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Observation of low heat capacities for vapor-deposited glasses of indomethacin as determined by AC nanocalorimetry
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Broadband Dielectric Relaxation Study at Ambient and Elevated Pressure of Molecular Dynamics of Pharmaceutical: Indomethacin
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The Temperature Dependence of Relaxation Mechanisms in Amorphous Polymers and Other Glass-forming Liquids
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On the surface of glasses
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Surface Self-Diffusion of Organic Glasses
journal, August 2013

Some quantum weirdness in physiology
journal, October 2009

Molecular view of the isothermal transformation of a stable glass to a liquid
journal, June 2008

Equilibrium ultrastable glasses produced by random pinning
journal, December 2014

Transformation kinetics of vapor-deposited thin film organic glasses: the role of stability and molecular packing anisotropy
journal, January 2015

Phase separation during bulk polymerization of methyl methacrylate
journal, November 2018

Perspective: Highly stable vapor-deposited glasses
journal, December 2017

Glass softening kinetics in the limit of high heating rates
journal, March 2019

Surface-Bulk Interplay in Vapor-Deposited Glasses: Crossover Length and the Origin of Front Transformation
journal, October 2019

Front-Mediated Melting of Isotropic Ultrastable Glasses
journal, October 2019