Disconnecting structure and dynamics in glassy thin films

Sussman, Daniel M.; Schoenholz, Samuel S.; Cubuk, Ekin D.; Liu, Andrea J.

doi:10.1073/pnas.1703927114

Title: Disconnecting structure and dynamics in glassy thin films

Abstract

Nanometrically thin glassy films depart strikingly from the behavior of their bulk counterparts. We investigate whether the dynamical differences between a bulk and thin film polymeric glass former can be understood by differences in local microscopic structure. Machine learning methods have shown that local structure can serve as the foundation for successful, predictive models of particle rearrangement dynamics in bulk systems. By contrast, in thin glassy films, we find that particles at the center of the film and those near the surface are structurally indistinguishable despite exhibiting very different dynamics. Next, we show that structure-independent processes, already present in bulk systems and demonstrably different from simple facilitated dynamics, are crucial for understanding glassy dynamics in thin films. Our analysis suggests a picture of glassy dynamics in which two dynamical processes coexist, with relative strengths that depend on the distance from an interface. Here, one of these processes depends on local structure and is unchanged throughout most of the film, while the other is purely Arrhenius, does not depend on local structure, and is strongly enhanced near the free surface of a film.

Authors:

Sussman, Daniel M. ^[1];

^[2]; Cubuk, Ekin D. ^[3]; Liu, Andrea J. ^[4]

Syracuse Univ., Syracuse, NY (United States)
Google, Mountain View, CA (United States)
Stanford Univ., Stanford, CA (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States)

Publication Date:: Tue Sep 19 00:00:00 EDT 2017

Research Org.:: Univ. of Pennsylvania, Philadelphia, PA (United States)

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

OSTI Identifier:: 1540262

Alternate Identifier(s):: OSTI ID: 1856741

Grant/Contract Number:: FG02-05ER46199

Resource Type:: Accepted Manuscript

Journal Name:: Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:: Journal Volume: 114; Journal Issue: 40; Journal ID: ISSN 0027-8424

Publisher:: National Academy of Sciences

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Science & Technology; Other Topics; machine learning; glass; thin film; Glass transition, glasses, thin films

Citation Formats


                    Sussman, Daniel M., Schoenholz, Samuel S., Cubuk, Ekin D., and Liu, Andrea J. Disconnecting structure and dynamics in glassy thin films.  United States: N. p., 2017. 
Web.  doi:10.1073/pnas.1703927114.

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                    Sussman, Daniel M., Schoenholz, Samuel S., Cubuk, Ekin D., & Liu, Andrea J. Disconnecting structure and dynamics in glassy thin films.  United States.  https://doi.org/10.1073/pnas.1703927114

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                    Sussman, Daniel M., Schoenholz, Samuel S., Cubuk, Ekin D., and Liu, Andrea J. Tue .  
"Disconnecting structure and dynamics in glassy thin films".  United States.  https://doi.org/10.1073/pnas.1703927114.  https://www.osti.gov/servlets/purl/1540262.

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@article{osti_1540262,

  title        = {Disconnecting structure and dynamics in glassy thin films},

  author       = {Sussman, Daniel M. and Schoenholz, Samuel S. and Cubuk, Ekin D. and Liu, Andrea J.},

  abstractNote = {Nanometrically thin glassy films depart strikingly from the behavior of their bulk counterparts. We investigate whether the dynamical differences between a bulk and thin film polymeric glass former can be understood by differences in local microscopic structure. Machine learning methods have shown that local structure can serve as the foundation for successful, predictive models of particle rearrangement dynamics in bulk systems. By contrast, in thin glassy films, we find that particles at the center of the film and those near the surface are structurally indistinguishable despite exhibiting very different dynamics. Next, we show that structure-independent processes, already present in bulk systems and demonstrably different from simple facilitated dynamics, are crucial for understanding glassy dynamics in thin films. Our analysis suggests a picture of glassy dynamics in which two dynamical processes coexist, with relative strengths that depend on the distance from an interface. Here, one of these processes depends on local structure and is unchanged throughout most of the film, while the other is purely Arrhenius, does not depend on local structure, and is strongly enhanced near the free surface of a film.},

  doi          = {10.1073/pnas.1703927114},

  journal      = {Proceedings of the National Academy of Sciences of the United States of America},

  number       = 40,

  volume       = 114,

  place        = {United States},

  year         = {Tue Sep 19 00:00:00 EDT 2017},

  month        = {Tue Sep 19 00:00:00 EDT 2017}

}

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Machine Learning Bell Nonlocality in Quantum Many-body Systems
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Deng, Dong-Ling
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Autonomous data-driven design of inorganic materials with AFLOW
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Speck, Thomas
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Title: Disconnecting structure and dynamics in glassy thin films

Abstract

Citation Formats

Cooperative motion and growing length scales in supercooled confined liquids journal, September 2002

Cooperative Strings and Glassy Interfaces text, January 2015

Cooperative strings and glassy interfaces journal, June 2015

Structure and dynamics in glass-formers: predictability at large length scales text, January 2007

Crossovers in the dynamics of supercooled liquids probed by an amorphous wall journal, May 2014

A Direct Quantitative Measure of Surface Mobility in a Glassy Polymer journal, February 2014

Lattice model of mobility at interfaces: free surfaces, substrates, and bilayers journal, January 2013

Measuring the Surface Dynamics of Glassy Polymers journal, February 2008

Identifying Structural Flow Defects in Disordered Solids Using Machine-Learning Methods journal, March 2015

Long-range correlated dynamics in ultra-thin molecular glass films journal, September 2016

Is the molecular surface of polystyrene really glassy? journal, September 1992

Vibrational Modes Identify Soft Spots in a Sheared Disordered Packing journal, August 2011

Direct Measurement of Molecular Motion in Freestanding Polystyrene Thin Films journal, June 2011

Decoupling of surface diffusion and relaxation dynamics of molecular glasses journal, April 2017

Discrete mobility on the surface of glasses journal, April 2017

Ensemble fluctuations matter for variances of macroscopic variables journal, February 2021

Cooperative motion and growing length scales in supercooled confined liquids text, January 2002

Dynamics near Free Surfaces and the Glass Transition in Thin Polymer Films: A View to the Future journal, November 2013

Spatial distribution of entanglements in thin free-standing films journal, July 2016

Interfacial Dynamic Length Scales in the Glass Transition of a Model Freestanding Polymer Film and Their Connection to Cooperative Motion journal, December 2013

Facilitation of interfacial dynamics in entangled polymer films journal, November 2014

Identifying structural flow defects in disordered solids using machine learning methods text, January 2014

Physical Aging, the Local Dynamics of Glass-Forming Polymers under Nanoscale Confinement journal, July 2014

Structural Properties of Defects in Glassy Liquids journal, April 2016

Physical Aging in Ultrathin Polystyrene Films: Evidence of a Gradient in Dynamics at the Free Surface and Its Connection to the Glass Transition Temperature Reductions journal, October 2010

Macroscopic Facilitation of Glassy Relaxation Kinetics: Ultra Stable Glass Films with Front-Like Thermal Response text, January 2010

A unifying framework to quantify the effects of substrate interactions, stiffness, and roughness on the dynamics of thin supported polymer films journal, June 2015

Building Blocks of Dynamical Heterogeneities in Dense Granular Media journal, February 2009

Non-monotonic temperature evolution of dynamic correlations in glass-forming liquids journal, October 2011

Glass Transition Dynamics and Surface Layer Mobility in Unentangled Polystyrene Films journal, June 2010

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

Interfacial mobility scale determines the scale of collective motion and relaxation rate in polymer films journal, June 2014

General purpose molecular dynamics simulations fully implemented on graphics processing units journal, May 2008

Crossovers in the dynamics of supercooled liquids probed by an amorphous wall text, January 2014

Equilibration of long chain polymer melts in computer simulations journal, December 2003

Influence of Backbone Rigidity on Nanoscale Confinement Effects in Model Glass-Forming Polymers journal, June 2013

A direct quantitative measure of surface mobility in a glassy polymer text, January 2014

Dynamics on the Way to Forming Glass: Bubbles in Space-Time journal, March 2010

Theory of activated glassy relaxation, mobility gradients, surface diffusion, and vitrification in free standing thin films journal, December 2015

Measurement of growing dynamical length scales and prediction of the jamming transition in a granular material journal, March 2007

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

Structure and dynamics of glass formers: Predictability at large length scales journal, October 2007

Direct observation of a local structural mechanism for dynamic arrest journal, June 2008

On the surface of glasses journal, December 2008

The building blocks of dynamical heterogeneities in dense granular media text, January 2008

Irreversible reorganization in a supercooled liquid originates from localized soft modes journal, July 2008

A structural approach to relaxation in glassy liquids journal, February 2016

Relationship between local structure and relaxation in out-of-equilibrium glassy systems journal, December 2016

Machine learning determination of atomic dynamics at grain boundaries journal, October 2018

Theory of the spatial transfer of interface-nucleated changes of dynamical constraints and its consequences in glass-forming films journal, January 2019

Attractive versus truncated repulsive supercooled liquids: The dynamics is encoded in the pair correlation function journal, January 2020

Machine Learning in a data-limited regime: Augmenting experiments with synthetic data uncovers order in crumpled sheets text, January 2018

Theory of the Spatial Transfer of Interface-Nucleated Changes of Dynamical Constraints and Its Consequences in Glass-Forming Films text, January 2019

Effect of substrate interactions on the glass transition and length-scale of correlated dynamics in ultra-thin molecular glass films journal, November 2018

Comparison of single particle dynamics at the center and on the surface of equilibrium glassy films journal, August 2018

Progress towards a phenomenological picture and theoretical understanding of glassy dynamics and vitrification near interfaces and under nanoconfinement journal, December 2019

Machine learning characterization of structural defects in amorphous packings of dimers and ellipses journal, February 2019

Machine learning determination of atomic dynamics at grain boundaries text, January 2018

Deep Learning for Automated Classification and Characterization of Amorphous Materials preprint, January 2019

Attractive versus truncated repulsive supercooled liquids: The dynamics is encoded in the pair correlation function text, January 2019

Machine learning in a data-limited regime: Augmenting experiments with synthetic data uncovers order in crumpled sheets journal, April 2019

Identifying structural signatures of shear banding in model polymer nanopillars journal, January 2019

Machine Learning Characterization of Structural Defects in Amorphous Packings of Dimers and Ellipses text, January 2018

Heterogeneous Activation, Local Structure, and Softness in Supercooled Colloidal Liquids journal, January 2019

Structure-property relationships from universal signatures of plasticity in disordered solids journal, November 2017

Unveiling the predictive power of static structure in glassy systems journal, April 2020

Correlating fragility and heterogeneous dynamics in polystyrene through single molecule studies journal, August 2019

Deep learning for automated classification and characterization of amorphous materials journal, January 2020

Uncovering the effects of interface-induced ordering of liquid on crystal growth using machine learning journal, June 2020

Mutual information, neural networks and the renormalization group journal, March 2018

A characteristic energy scale in glasses journal, June 2018

Spin-qubit noise spectroscopy from randomized benchmarking by supervised learning journal, April 2019

Collective diffusion within the superionic regime of Bi2O3 journal, March 2020

Transition from stress-driven to thermally activated stress relaxation in metallic glasses journal, September 2016

Learning thermodynamics with Boltzmann machines journal, October 2016

Few-shot machine learning in the three-dimensional Ising model journal, March 2019

Attractive versus truncated repulsive supercooled liquids: The dynamics is encoded in the pair correlation function journal, January 2020

Cooperative motion and growing length scales in supercooled confined liquids
journal, September 2002

Cooperative Strings and Glassy Interfaces
text, January 2015

Cooperative strings and glassy interfaces
journal, June 2015

Structure and dynamics in glass-formers: predictability at large length scales
text, January 2007

Crossovers in the dynamics of supercooled liquids probed by an amorphous wall
journal, May 2014

A Direct Quantitative Measure of Surface Mobility in a Glassy Polymer
journal, February 2014

Lattice model of mobility at interfaces: free surfaces, substrates, and bilayers
journal, January 2013

Measuring the Surface Dynamics of Glassy Polymers
journal, February 2008

Identifying Structural Flow Defects in Disordered Solids Using Machine-Learning Methods
journal, March 2015

Long-range correlated dynamics in ultra-thin molecular glass films
journal, September 2016

Is the molecular surface of polystyrene really glassy?
journal, September 1992

Vibrational Modes Identify Soft Spots in a Sheared Disordered Packing
journal, August 2011

Direct Measurement of Molecular Motion in Freestanding Polystyrene Thin Films
journal, June 2011

Decoupling of surface diffusion and relaxation dynamics of molecular glasses
journal, April 2017

Discrete mobility on the surface of glasses
journal, April 2017

Ensemble fluctuations matter for variances of macroscopic variables
journal, February 2021

Cooperative motion and growing length scales in supercooled confined liquids
text, January 2002

Dynamics near Free Surfaces and the Glass Transition in Thin Polymer Films: A View to the Future
journal, November 2013

Spatial distribution of entanglements in thin free-standing films
journal, July 2016

Interfacial Dynamic Length Scales in the Glass Transition of a Model Freestanding Polymer Film and Their Connection to Cooperative Motion
journal, December 2013

Facilitation of interfacial dynamics in entangled polymer films
journal, November 2014

Identifying structural flow defects in disordered solids using machine learning methods
text, January 2014

Physical Aging, the Local Dynamics of Glass-Forming Polymers under Nanoscale Confinement
journal, July 2014

Structural Properties of Defects in Glassy Liquids
journal, April 2016

Physical Aging in Ultrathin Polystyrene Films: Evidence of a Gradient in Dynamics at the Free Surface and Its Connection to the Glass Transition Temperature Reductions
journal, October 2010

Macroscopic Facilitation of Glassy Relaxation Kinetics: Ultra Stable Glass Films with Front-Like Thermal Response
text, January 2010

A unifying framework to quantify the effects of substrate interactions, stiffness, and roughness on the dynamics of thin supported polymer films
journal, June 2015

Building Blocks of Dynamical Heterogeneities in Dense Granular Media
journal, February 2009

Non-monotonic temperature evolution of dynamic correlations in glass-forming liquids
journal, October 2011

Glass Transition Dynamics and Surface Layer Mobility in Unentangled Polystyrene Films
journal, June 2010

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

Interfacial mobility scale determines the scale of collective motion and relaxation rate in polymer films
journal, June 2014

General purpose molecular dynamics simulations fully implemented on graphics processing units
journal, May 2008

Crossovers in the dynamics of supercooled liquids probed by an amorphous wall
text, January 2014

Equilibration of long chain polymer melts in computer simulations
journal, December 2003

Influence of Backbone Rigidity on Nanoscale Confinement Effects in Model Glass-Forming Polymers
journal, June 2013

A direct quantitative measure of surface mobility in a glassy polymer
text, January 2014

Dynamics on the Way to Forming Glass: Bubbles in Space-Time
journal, March 2010

Theory of activated glassy relaxation, mobility gradients, surface diffusion, and vitrification in free standing thin films
journal, December 2015

Measurement of growing dynamical length scales and prediction of the jamming transition in a granular material
journal, March 2007

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

Structure and dynamics of glass formers: Predictability at large length scales
journal, October 2007

Direct observation of a local structural mechanism for dynamic arrest
journal, June 2008

On the surface of glasses
journal, December 2008

The building blocks of dynamical heterogeneities in dense granular media
text, January 2008

Irreversible reorganization in a supercooled liquid originates from localized soft modes
journal, July 2008

A structural approach to relaxation in glassy liquids
journal, February 2016

Relationship between local structure and relaxation in out-of-equilibrium glassy systems
journal, December 2016

Machine learning determination of atomic dynamics at grain boundaries
journal, October 2018

Theory of the spatial transfer of interface-nucleated changes of dynamical constraints and its consequences in glass-forming films
journal, January 2019

Attractive versus truncated repulsive supercooled liquids: The dynamics is encoded in the pair correlation function
journal, January 2020

Machine Learning in a data-limited regime: Augmenting experiments with synthetic data uncovers order in crumpled sheets
text, January 2018

Theory of the Spatial Transfer of Interface-Nucleated Changes of Dynamical Constraints and Its Consequences in Glass-Forming Films
text, January 2019

Effect of substrate interactions on the glass transition and length-scale of correlated dynamics in ultra-thin molecular glass films
journal, November 2018

Comparison of single particle dynamics at the center and on the surface of equilibrium glassy films
journal, August 2018

Progress towards a phenomenological picture and theoretical understanding of glassy dynamics and vitrification near interfaces and under nanoconfinement
journal, December 2019

Machine learning characterization of structural defects in amorphous packings of dimers and ellipses
journal, February 2019

Machine learning determination of atomic dynamics at grain boundaries
text, January 2018

Deep Learning for Automated Classification and Characterization of Amorphous Materials
preprint, January 2019

Attractive versus truncated repulsive supercooled liquids: The dynamics is encoded in the pair correlation function
text, January 2019

Machine learning in a data-limited regime: Augmenting experiments with synthetic data uncovers order in crumpled sheets
journal, April 2019

Identifying structural signatures of shear banding in model polymer nanopillars
journal, January 2019

Machine Learning Characterization of Structural Defects in Amorphous Packings of Dimers and Ellipses
text, January 2018

Heterogeneous Activation, Local Structure, and Softness in Supercooled Colloidal Liquids
journal, January 2019

Structure-property relationships from universal signatures of plasticity in disordered solids
journal, November 2017

Unveiling the predictive power of static structure in glassy systems
journal, April 2020

Correlating fragility and heterogeneous dynamics in polystyrene through single molecule studies
journal, August 2019

Deep learning for automated classification and characterization of amorphous materials
journal, January 2020

Uncovering the effects of interface-induced ordering of liquid on crystal growth using machine learning
journal, June 2020

Mutual information, neural networks and the renormalization group
journal, March 2018

A characteristic energy scale in glasses
journal, June 2018

Spin-qubit noise spectroscopy from randomized benchmarking by supervised learning
journal, April 2019

Collective diffusion within the superionic regime of Bi2O3
journal, March 2020

Transition from stress-driven to thermally activated stress relaxation in metallic glasses
journal, September 2016

Learning thermodynamics with Boltzmann machines
journal, October 2016

Few-shot machine learning in the three-dimensional Ising model
journal, March 2019

Attractive versus truncated repulsive supercooled liquids: The dynamics is encoded in the pair correlation function
journal, January 2020

Nonequilibrium thermodynamics of restricted Boltzmann machines
journal, August 2017

Local yield stress statistics in model amorphous solids
journal, March 2018

Matrix product operators for sequence-to-sequence learning
journal, October 2018