Connectivity and free-surface effects in polymer glasses

Lappala, Anna; Sefton, Luke; Fenimore, Paul; Terentjev, Eugene

doi:10.1038/s41598-019-40286-2

Title: Connectivity and free-surface effects in polymer glasses

Abstract

The glass transition is one of the few unsolved problems in condensed matter physics: agreement on the cause of the slowing down of structural relaxation in glass-forming liquids is lacking. Glasses are amorphous solids, which do not possess the long-range crystalline order, yet display arrested dynamics and the shear elastic modulus characteristic of equilibrium elasticity. It has been suggested that due to the influence of intramolecular interactions and chain connectivity, the nature of the glass transition in polymers and in standard glass-formers is fundamentally different. Here, we discuss the role of connectivity in polymer glasses, demonstrating that although covalent bonding promotes glass formation, bonding sequentiality that defines a polymer chain is not critical in the bulk: glassy dynamics is purely a result of the number of connections per particle, independently of how these connections are formed, agreeing with the classical Phillips-Thorpe topological constraint theory. We show that bonding sequentiality does play an important role in the surface effects of the glass, highlighting a major difference between polymeric and colloidal glasses. Further, we identify the heterogenous dynamics of model coarse-grained polymer chains both in ‘bulk’ and near the free surface, and demonstrate characteristic domain patterns in local displacement and connectivity.

Authors:

^[1]; Sefton, Luke ^[2]; Fenimore, Paul ^[1]; Terentjev, Eugene ^[2]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of Cambridge (United Kingdom)

Publication Date:: Thu Mar 07 00:00:00 EST 2019

Research Org.:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1501808

Report Number(s):: LA-UR-18-25676
Journal ID: ISSN 2045-2322

Grant/Contract Number:: 89233218CNA000001

Resource Type:: Accepted Manuscript

Journal Name:: Scientific Reports

Additional Journal Information:: Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2045-2322

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats


                    Lappala, Anna, Sefton, Luke, Fenimore, Paul, and Terentjev, Eugene. Connectivity and free-surface effects in polymer glasses.  United States: N. p., 2019. 
Web.  doi:10.1038/s41598-019-40286-2.

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                    Lappala, Anna, Sefton, Luke, Fenimore, Paul, & Terentjev, Eugene. Connectivity and free-surface effects in polymer glasses.  United States.  https://doi.org/10.1038/s41598-019-40286-2

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                    Lappala, Anna, Sefton, Luke, Fenimore, Paul, and Terentjev, Eugene. Thu .  
"Connectivity and free-surface effects in polymer glasses".  United States.  https://doi.org/10.1038/s41598-019-40286-2.  https://www.osti.gov/servlets/purl/1501808.

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@article{osti_1501808,

  title        = {Connectivity and free-surface effects in polymer glasses},

  author       = {Lappala, Anna and Sefton, Luke and Fenimore, Paul and Terentjev, Eugene},

  abstractNote = {The glass transition is one of the few unsolved problems in condensed matter physics: agreement on the cause of the slowing down of structural relaxation in glass-forming liquids is lacking. Glasses are amorphous solids, which do not possess the long-range crystalline order, yet display arrested dynamics and the shear elastic modulus characteristic of equilibrium elasticity. It has been suggested that due to the influence of intramolecular interactions and chain connectivity, the nature of the glass transition in polymers and in standard glass-formers is fundamentally different. Here, we discuss the role of connectivity in polymer glasses, demonstrating that although covalent bonding promotes glass formation, bonding sequentiality that defines a polymer chain is not critical in the bulk: glassy dynamics is purely a result of the number of connections per particle, independently of how these connections are formed, agreeing with the classical Phillips-Thorpe topological constraint theory. We show that bonding sequentiality does play an important role in the surface effects of the glass, highlighting a major difference between polymeric and colloidal glasses. Further, we identify the heterogenous dynamics of model coarse-grained polymer chains both in ‘bulk’ and near the free surface, and demonstrate characteristic domain patterns in local displacement and connectivity.},

  doi          = {10.1038/s41598-019-40286-2},

  journal      = {Scientific Reports},

  number       = 1,

  volume       = 9,

  place        = {United States},

  year         = {Thu Mar 07 00:00:00 EST 2019},

  month        = {Thu Mar 07 00:00:00 EST 2019}

}

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Works referencing / citing this record:

Four-dimensional chromosome reconstruction elucidates the spatiotemporal reorganization of the mammalian X chromosome
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Lappala, Anna; Wang, Chen-Yu; Kriz, Andrea
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Title: Connectivity and free-surface effects in polymer glasses

Abstract

Citation Formats

Structure and Dynamics of Interphase Chromosomes journal, August 2008

Structure and Dynamics of Interphase Chromosomes journal, August 2008

Relaxation processes in supercooled liquids journal, March 1992

On the origin of dynamic heterogeneities in glass-forming liquids journal, December 1999

The Glass Transition of a Single Macromolecule journal, September 2016

Effect of chain stiffness on the competition between crystallization and glass-formation in model unentangled polymers journal, October 2015

Evidence of a Transition Layer between the Free Surface and the Bulk journal, February 2018

The Glass Transition of a Single Macromolecule journal, September 2016

Measuring the Surface Dynamics of Glassy Polymers journal, February 2008

Constraint theory, vector percolation and glass formation journal, February 1985

Polymer glass transition occurs at the marginal rigidity point with connectivity z* = 4 journal, January 2016

Effect of chain stiffness on the competition between crystallization and glass-formation in model unentangled polymers journal, October 2015

Cooling rate dependence of the glass transition temperature of polymer melts: Molecular dynamics study journal, October 2002

The Surface Mobility of Glasses journal, February 2014

Arrested Spinodal Decomposition in Polymer Brush Collapsing in Poor Solvent journal, March 2015

50th Anniversary Perspective : Polymer Conformation—A Pedagogical Review journal, November 2017

Heterogeneity at the glass transition: a review journal, February 1999

Glass transition of polymers in bulk, confined geometries, and near interfaces journal, January 2017

Relaxation processes in supercooled liquids journal, March 1992

Polymer-specific effects of bulk relaxation and stringlike correlated motion in the dynamics of a supercooled polymer melt journal, September 2003

On the origin of dynamic heterogeneities in glass-forming liquids journal, December 1999

Dynamics of a supercooled polymer melt above the mode-coupling critical temperature: cage versus polymer-specific effects journal, July 2000

Direct Experimental Evidence of a Growing Length Scale Accompanying the Glass Transition journal, December 2005

Glass transition of polymers in bulk, confined geometries, and near interfaces journal, January 2017

S PATIALLY H ETEROGENEOUS D YNAMICS IN S UPERCOOLED L IQUIDS journal, October 2000

Spatially heterogeneous dynamics in liquids: insights from simulation journal, September 2000

Dynamics of entangled linear polymer melts: A molecular‐dynamics simulation journal, April 1990

Quantifying spatially heterogeneous dynamics in computer simulations of glass-forming liquids journal, January 1999

Molecular dynamics study of binary soft‐sphere mixtures: Jump motions of atoms in the glassy state journal, March 1988

Character of the glass transition in thin supported polymer films journal, January 2001

Measuring the Surface Dynamics of Glassy Polymers journal, February 2008

Molecular dynamics study of binary soft‐sphere mixtures: Jump motions of atoms in the glassy state journal, March 1988

Evidence of a Transition Layer between the Free Surface and the Bulk journal, February 2018

Dynamics of a supercooled polymer melt above the mode-coupling critical temperature: cage versus polymer-specific effects journal, July 2000

Reduced Glass Transition Temperatures in Thin Polymer Films: Surface Effect or Artifact? journal, August 2012

Cooling rate dependence of the glass transition temperature of polymer melts: Molecular dynamics study journal, October 2002

50th Anniversary Perspective : Polymer Conformation—A Pedagogical Review journal, November 2017

Dynamics of entangled linear polymer melts: A molecular‐dynamics simulation journal, April 1990

Constraint theory, vector percolation and glass formation journal, February 1985

S PATIALLY H ETEROGENEOUS D YNAMICS IN S UPERCOOLED L IQUIDS journal, October 2000

Deeper penetration of surface effects on particle mobility than on hopping rate in glassy polymer films journal, October 2018

Four-dimensional chromosome reconstruction elucidates the spatiotemporal reorganization of the mammalian X chromosome journal, October 2021

Structure and Dynamics of Interphase Chromosomes
journal, August 2008

Structure and Dynamics of Interphase Chromosomes
journal, August 2008

Relaxation processes in supercooled liquids
journal, March 1992

On the origin of dynamic heterogeneities in glass-forming liquids
journal, December 1999

The Glass Transition of a Single Macromolecule
journal, September 2016

Effect of chain stiffness on the competition between crystallization and glass-formation in model unentangled polymers
journal, October 2015

Evidence of a Transition Layer between the Free Surface and the Bulk
journal, February 2018

The Glass Transition of a Single Macromolecule
journal, September 2016

Measuring the Surface Dynamics of Glassy Polymers
journal, February 2008

Constraint theory, vector percolation and glass formation
journal, February 1985

Polymer glass transition occurs at the marginal rigidity point with connectivity z* = 4
journal, January 2016

Effect of chain stiffness on the competition between crystallization and glass-formation in model unentangled polymers
journal, October 2015

Cooling rate dependence of the glass transition temperature of polymer melts: Molecular dynamics study
journal, October 2002

The Surface Mobility of Glasses
journal, February 2014

Arrested Spinodal Decomposition in Polymer Brush Collapsing in Poor Solvent
journal, March 2015

50th Anniversary Perspective : Polymer Conformation—A Pedagogical Review
journal, November 2017

Heterogeneity at the glass transition: a review
journal, February 1999

Glass transition of polymers in bulk, confined geometries, and near interfaces
journal, January 2017

Relaxation processes in supercooled liquids
journal, March 1992

Polymer-specific effects of bulk relaxation and stringlike correlated motion in the dynamics of a supercooled polymer melt
journal, September 2003

On the origin of dynamic heterogeneities in glass-forming liquids
journal, December 1999

Dynamics of a supercooled polymer melt above the mode-coupling critical temperature: cage versus polymer-specific effects
journal, July 2000

Direct Experimental Evidence of a Growing Length Scale Accompanying the Glass Transition
journal, December 2005

Glass transition of polymers in bulk, confined geometries, and near interfaces
journal, January 2017

S PATIALLY H ETEROGENEOUS D YNAMICS IN S UPERCOOLED L IQUIDS
journal, October 2000

Spatially heterogeneous dynamics in liquids: insights from simulation
journal, September 2000

Dynamics of entangled linear polymer melts: A molecular‐dynamics simulation
journal, April 1990

Quantifying spatially heterogeneous dynamics in computer simulations of glass-forming liquids
journal, January 1999

Molecular dynamics study of binary soft‐sphere mixtures: Jump motions of atoms in the glassy state
journal, March 1988

Character of the glass transition in thin supported polymer films
journal, January 2001

Measuring the Surface Dynamics of Glassy Polymers
journal, February 2008

Molecular dynamics study of binary soft‐sphere mixtures: Jump motions of atoms in the glassy state
journal, March 1988

Evidence of a Transition Layer between the Free Surface and the Bulk
journal, February 2018

Dynamics of a supercooled polymer melt above the mode-coupling critical temperature: cage versus polymer-specific effects
journal, July 2000

Reduced Glass Transition Temperatures in Thin Polymer Films: Surface Effect or Artifact?
journal, August 2012

Cooling rate dependence of the glass transition temperature of polymer melts: Molecular dynamics study
journal, October 2002

50th Anniversary Perspective : Polymer Conformation—A Pedagogical Review
journal, November 2017

Dynamics of entangled linear polymer melts: A molecular‐dynamics simulation
journal, April 1990

Constraint theory, vector percolation and glass formation
journal, February 1985

S PATIALLY H ETEROGENEOUS D YNAMICS IN S UPERCOOLED L IQUIDS
journal, October 2000

Deeper penetration of surface effects on particle mobility than on hopping rate in glassy polymer films
journal, October 2018

Four-dimensional chromosome reconstruction elucidates the spatiotemporal reorganization of the mammalian X chromosome
journal, October 2021