Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids

Jaiswal, Abhishek; Egami, Takeshi; Kelton, K. F.; Schweizer, Kenneth S.; Zhang, Yang

doi:10.1103/PhysRevLett.117.205701

Title: Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids

Abstract

In this paper, we report the observation of a distinct correlation between the kinetic fragility index m and the reduced Arrhenius crossover temperature θ_A = T_A/T_g in various glass-forming liquids, identifying three distinguishable groups. In particular, for 11 glass-forming metallic liquids, we universally observe a crossover in the mean diffusion coefficient from high-temperature Arrhenius to low-temperature super-Arrhenius behavior at approximately θ_A ≈ 2 which is in the stable liquid phases. In contrast, for fragile molecular liquids, this crossover occurs at much lower θ_A ≈ 1.4 and usually in their supercooled states. The θ_A values for strong network liquids spans a wide range higher than 2. Intriguingly, the high-temperature activation barrier E_∞ is universally found to be ~11k_BT_g and uncorrelated with the fragility or the reduced crossover temperature θ_A for metallic and molecular liquids. Finally, these observations provide a way to estimate the low-temperature glassy characteristics (T_g and m) from the high-temperature liquid quantities (E_∞ and θ_A).

Authors:

Jaiswal, Abhishek ^[1]; Egami, Takeshi ^[2]; Kelton, K. F. ^[3]; Schweizer, Kenneth S. ^[4]; Zhang, Yang ^[5]

Univ. of Illinois, Urbana, IL (United States). Dept. of Nuclear, Plasma, and Radiological Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Washington Univ., St. Louis, MO (United States). Dept. of Physics. Inst. of Materials Science and Engineering
Univ. of Illinois, Urbana, IL (United States). Dept. of Materials Science and Engineering
Univ. of Illinois, Urbana, IL (United States). Dept. of Nuclear, Plasma, and Radiological Engineering. Dept. of Materials Science and Engineering

Publication Date:: Thu Nov 10 00:00:00 EST 2016

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Illinois at Urbana-Champaign, IL (United States)

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

Contributing Org.:: Univ. of Tennessee, Knoxville, TN (United States); Washington Univ., St. Louis, MO (United States)

OSTI Identifier:: 1337816

Alternate Identifier(s):: OSTI ID: 1331724

Grant/Contract Number:: SC0014804; SC-0014804

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Letters

Additional Journal Information:: Journal Volume: 117; Journal Issue: 20; Journal ID: ISSN 0031-9007

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Jaiswal, Abhishek, Egami, Takeshi, Kelton, K. F., Schweizer, Kenneth S., and Zhang, Yang. Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids.  United States: N. p., 2016. 
Web.  doi:10.1103/PhysRevLett.117.205701.

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                    Jaiswal, Abhishek, Egami, Takeshi, Kelton, K. F., Schweizer, Kenneth S., & Zhang, Yang. Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids.  United States.  https://doi.org/10.1103/PhysRevLett.117.205701

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                    Jaiswal, Abhishek, Egami, Takeshi, Kelton, K. F., Schweizer, Kenneth S., and Zhang, Yang. Thu .  
"Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids".  United States.  https://doi.org/10.1103/PhysRevLett.117.205701.  https://www.osti.gov/servlets/purl/1337816.

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@article{osti_1337816,

  title        = {Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids},

  author       = {Jaiswal, Abhishek and Egami, Takeshi and Kelton, K. F. and Schweizer, Kenneth S. and Zhang, Yang},

  abstractNote = {In this paper, we report the observation of a distinct correlation between the kinetic fragility index m and the reduced Arrhenius crossover temperature θA = TA/Tg in various glass-forming liquids, identifying three distinguishable groups. In particular, for 11 glass-forming metallic liquids, we universally observe a crossover in the mean diffusion coefficient from high-temperature Arrhenius to low-temperature super-Arrhenius behavior at approximately θA ≈ 2 which is in the stable liquid phases. In contrast, for fragile molecular liquids, this crossover occurs at much lower θA ≈ 1.4 and usually in their supercooled states. The θA values for strong network liquids spans a wide range higher than 2. Intriguingly, the high-temperature activation barrier E∞ is universally found to be ~11kBTg and uncorrelated with the fragility or the reduced crossover temperature θA for metallic and molecular liquids. Finally, these observations provide a way to estimate the low-temperature glassy characteristics (Tg and m) from the high-temperature liquid quantities (E∞ and θA).},

  doi          = {10.1103/PhysRevLett.117.205701},

  journal      = {Physical Review Letters},

  number       = 20,

  volume       = 117,

  place        = {United States},

  year         = {Thu Nov 10 00:00:00 EST 2016},

  month        = {Thu Nov 10 00:00:00 EST 2016}

}

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Physical Review B, Vol. 101, Issue 1
DOI: 10.1103/physrevb.101.014207

Resistivity Saturation in Metallic Liquids Above a Dynamical Crossover Temperature Observed in Measurements Aboard the International Space Station
journal, November 2019

Van Hoesen, D. C.; Gangopadhyay, A. K.; Lohöfer, G.
Physical Review Letters, Vol. 123, Issue 22
DOI: 10.1103/physrevlett.123.226601

Effects of dopants on the glass forming ability in Al-based metallic alloy
journal, February 2019

Sun, Yang; Zhang, Feng; Yang, Lin
Physical Review Materials, Vol. 3, Issue 2
DOI: 10.1103/physrevmaterials.3.023404

Effects of Dopants on the Glass Forming Ability in Al-Based Metallic Alloy
journal, January 2018

Ph. D., Yang Sun,; Zhang, Feng; Yang, Lin
SSRN Electronic Journal
DOI: 10.2139/ssrn.3289659

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Title: Correlation between Fragility and the Arrhenius Crossover Phenomenon in Metallic, Molecular, and Network Liquids

Abstract

Citation Formats

Dynamics in Cu46Zr42Al7Y5 melts: Interplay between packing density and viscosity journal, May 2009

The β relaxation in metallic glasses: an overview journal, May 2013

Correlation of fragility and Poisson’s ratio: Difference between metallic and nonmetallic glass formers journal, August 2006

Corresponding States of Structural Glass Formers journal, April 2009

The viscous slowing down of supercooled liquids as a temperature-controlled super-Arrhenius activated process: a description in terms of frustration-limited domains journal, July 2000

A structural signature of liquid fragility journal, August 2014

Coupled relaxation processes in a glass forming ZrTiNiCuBe liquid journal, July 2014

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Theoretical perspective on the glass transition and amorphous materials journal, June 2011

Thermophysical properties of a Cu46Zr42Al7Y5 bulk metallic glass-forming liquid journal, May 2006

On the correlation between fragility and stretching in glass-forming liquids journal, January 2007

Enthalpy Relaxation upon Glass Transition and Kinetic Fragility of Molecular Liquids journal, April 2009

Spatially Heterogeneous Dynamics and Dynamic Facilitation in a Model of Viscous Silica journal, June 2004

Time-Temperature Superposition of Structural Relaxation in a Viscous Metallic Liquid journal, December 1999

Fragility and thermodynamics in nonpolymeric glass-forming liquids journal, August 2006

Transport properties of glass-forming liquids suggest that dynamic crossover temperature is as important as the glass transition temperature journal, December 2010

Compilation of the fragility parameters for several glass-forming metallic alloys journal, January 1999

Thermophysical properties of Ni–Nb and Ni–Nb–Sn bulk metallic glass-forming melts by containerless electrostatic levitation processing journal, June 2004

Glassy dynamics and mechanical response in dense fluids of soft repulsive spheres. I. Activated relaxation, kinetic vitrification, and fragility journal, May 2011

Alloying strongly influences the structure, dynamics, and glass forming ability of metallic supercooled liquids journal, September 2008

Crossover to potential energy landscape dominated dynamics in a model glass-forming liquid journal, June 2000

Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid journal, February 2016

Fast diffusion in ZrTiCuNiBe melts journal, November 2003

Prevalence of approximate t relaxation for the dielectric α process in viscous organic liquids journal, April 2009

Correlation between fragility and glass-forming ability/plasticity in metallic glass-forming alloys journal, July 2007

Glass Transition Dynamics and Boiling Temperatures of Molecular Liquids and Their Isomers journal, March 2007

The β-relaxation in metallic glasses journal, June 2014

Fragility of network-forming glasses: A universal dependence on the topological connectivity journal, December 2015

The shapes of cooperatively rearranging regions in glass-forming liquids journal, March 2006

A brief overview of bulk metallic glasses journal, September 2011

Interatomic repulsion softness directly controls the fragility of supercooled metallic melts journal, October 2015

Viscosity, structure and mixing in (Ca, Na) silicate melts journal, May 2006

Relaxation in glassforming liquids and amorphous solids journal, September 2000

Broadband dielectric spectroscopy on benzophenone: α relaxation, β relaxation, and mode coupling theory journal, March 2008

On Poisson's ratio of glass and liquid vitrification characteristics journal, April 2006

The dynamics crossover region in phenol- and cresol-phthalein-dimethylethers under different conditions of pressure and temperature journal, March 2003

Dynamics of glass-forming liquids. XV. Dynamical features of molecular liquids that form ultra-stable glasses by vapor deposition journal, September 2011

Evolution of the dynamic susceptibility in molecular glass formers: Results from light scattering, dielectric spectroscopy, and NMR journal, March 2013

Divergent dynamics and the Kauzmann temperature in glass forming systems journal, June 2014

The dynamic susceptibility in glass forming molecular liquids: The search for universal relaxation patterns II journal, April 2006

Signatures of distinct dynamical regimes in the energy landscape of a glass-forming liquid journal, June 1998

Mechanical spectra of glass-forming liquids. II. Gigahertz-frequency longitudinal and shear acoustic dynamics in glycerol and DC704 studied by time-domain Brillouin scattering journal, March 2013

Temperature dependence of the Landau-Placzek ratio in glass forming liquids journal, October 2011

Complex atomic dynamics in a deep-eutectic binary metallic melt journal, October 2012

A “universal” criterion for metallic glass formation journal, June 2012

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

Decoupling of Component Diffusion in a Glass-Forming Zr 46.75 Ti 8.25 Cu 7.5 Ni 10 Be 27.5 Melt Far above the Liquidus Temperature journal, October 2014

Correlation between dynamic fragility and glass transition temperature for different classes of glass forming liquids journal, August 2006

Correlations between elastic moduli and properties in bulk metallic glasses journal, May 2006

Dynamic Singularity in Multicomponent Glass-Forming Metallic Liquids journal, July 2008

Pressure and temperature dependence of structural relaxation in diglycidylether of bisphenol A journal, February 2003

Correlation of fragility of supercooled liquids with elastic properties of glasses journal, June 2005

Stokes–Einstein relation in dense metallic glass-forming melts journal, November 2010

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Comment on “High-Frequency Dynamics in Metallic Glasses” journal, February 2007

Theory of non-linear susceptibility and correlation length in glasses and liquids journal, September 2002

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High-Frequency Dynamics in Metallic Glasses journal, April 2006

Poisson's ratio and the fragility of glass-forming liquids journal, October 2004

Atomic transport in dense multicomponent metallic liquids journal, October 2002

Two-step relaxation in a viscous metallic liquid journal, August 1999

Characteristic relaxation times and their invariance to thermodynamic conditions journal, January 2008

Proposal for universality in the viscosity of metallic liquids journal, September 2015

Theory of dynamic barriers, activated hopping, and the glass transition in polymer melts journal, July 2004

A macroscopic model that connects the molar excess entropy of a supercooled liquid near its glass transition temperature to its viscosity journal, November 2012

Universality of the dynamic crossover in glass-forming liquids: A “magic” relaxation time journal, March 2003

Atomic dynamics in binary Zr-Cu liquids journal, August 2014

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Correlation between fragility and cooperativity in bulk metallic glass-forming liquids journal, October 2010

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Fast and slow dynamics in Pr60Ni10Cu20Al10 melts as seen by neutron scattering journal, January 2008

Dynamic fragility in polymers: A comparison in isobaric and isochoric conditions journal, March 2002

Viscosity of titania-bearing sodium silicate melts journal, June 1996

Dynamics in Cu46Zr42Al7Y5 melts: Interplay between packing density and viscosity
journal, May 2009

The β relaxation in metallic glasses: an overview
journal, May 2013

Correlation of fragility and Poisson’s ratio: Difference between metallic and nonmetallic glass formers
journal, August 2006

Corresponding States of Structural Glass Formers
journal, April 2009

The viscous slowing down of supercooled liquids as a temperature-controlled super-Arrhenius activated process: a description in terms of frustration-limited domains
journal, July 2000

A structural signature of liquid fragility
journal, August 2014

Coupled relaxation processes in a glass forming ZrTiNiCuBe liquid
journal, July 2014

Structural evolution during fragile-to-strong transition in CuZr(Al) glass-forming liquids
journal, February 2015

Theoretical perspective on the glass transition and amorphous materials
journal, June 2011

Thermophysical properties of a Cu46Zr42Al7Y5 bulk metallic glass-forming liquid
journal, May 2006

On the correlation between fragility and stretching in glass-forming liquids
journal, January 2007

Enthalpy Relaxation upon Glass Transition and Kinetic Fragility of Molecular Liquids
journal, April 2009

Spatially Heterogeneous Dynamics and Dynamic Facilitation in a Model of Viscous Silica
journal, June 2004

Time-Temperature Superposition of Structural Relaxation in a Viscous Metallic Liquid
journal, December 1999

Fragility and thermodynamics in nonpolymeric glass-forming liquids
journal, August 2006

Transport properties of glass-forming liquids suggest that dynamic crossover temperature is as important as the glass transition temperature
journal, December 2010

Compilation of the fragility parameters for several glass-forming metallic alloys
journal, January 1999

Thermophysical properties of Ni–Nb and Ni–Nb–Sn bulk metallic glass-forming melts by containerless electrostatic levitation processing
journal, June 2004

Glassy dynamics and mechanical response in dense fluids of soft repulsive spheres. I. Activated relaxation, kinetic vitrification, and fragility
journal, May 2011

Alloying strongly influences the structure, dynamics, and glass forming ability of metallic supercooled liquids
journal, September 2008

Crossover to potential energy landscape dominated dynamics in a model glass-forming liquid
journal, June 2000

Onset of Cooperative Dynamics in an Equilibrium Glass-Forming Metallic Liquid
journal, February 2016

Fast diffusion in ZrTiCuNiBe melts
journal, November 2003

Prevalence of approximate t relaxation for the dielectric α process in viscous organic liquids
journal, April 2009

Correlation between fragility and glass-forming ability/plasticity in metallic glass-forming alloys
journal, July 2007

Glass Transition Dynamics and Boiling Temperatures of Molecular Liquids and Their Isomers
journal, March 2007

The β-relaxation in metallic glasses
journal, June 2014

Fragility of network-forming glasses: A universal dependence on the topological connectivity
journal, December 2015

The shapes of cooperatively rearranging regions in glass-forming liquids
journal, March 2006

A brief overview of bulk metallic glasses
journal, September 2011

Interatomic repulsion softness directly controls the fragility of supercooled metallic melts
journal, October 2015

Viscosity, structure and mixing in (Ca, Na) silicate melts
journal, May 2006

Relaxation in glassforming liquids and amorphous solids
journal, September 2000

Broadband dielectric spectroscopy on benzophenone: $α$ relaxation, $β$ relaxation, and mode coupling theory
journal, March 2008

On Poisson's ratio of glass and liquid vitrification characteristics
journal, April 2006

The dynamics crossover region in phenol- and cresol-phthalein-dimethylethers under different conditions of pressure and temperature
journal, March 2003

Dynamics of glass-forming liquids. XV. Dynamical features of molecular liquids that form ultra-stable glasses by vapor deposition
journal, September 2011

Evolution of the dynamic susceptibility in molecular glass formers: Results from light scattering, dielectric spectroscopy, and NMR
journal, March 2013

Divergent dynamics and the Kauzmann temperature in glass forming systems
journal, June 2014

The dynamic susceptibility in glass forming molecular liquids: The search for universal relaxation patterns II
journal, April 2006

Signatures of distinct dynamical regimes in the energy landscape of a glass-forming liquid
journal, June 1998

Mechanical spectra of glass-forming liquids. II. Gigahertz-frequency longitudinal and shear acoustic dynamics in glycerol and DC704 studied by time-domain Brillouin scattering
journal, March 2013

Temperature dependence of the Landau-Placzek ratio in glass forming liquids
journal, October 2011

Complex atomic dynamics in a deep-eutectic binary metallic melt
journal, October 2012

A “universal” criterion for metallic glass formation
journal, June 2012

Testing mode-coupling theory for a supercooled binary Lennard-Jones mixture I: The van Hove correlation function
journal, May 1995

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

Decoupling of Component Diffusion in a Glass-Forming ${Zr}_{46.75} {Ti}_{8.25} {Cu}_{7.5} {Ni}_{10} {Be}_{27.5}$ Melt Far above the Liquidus Temperature
journal, October 2014

Correlation between dynamic fragility and glass transition temperature for different classes of glass forming liquids
journal, August 2006

Correlations between elastic moduli and properties in bulk metallic glasses
journal, May 2006

Dynamic Singularity in Multicomponent Glass-Forming Metallic Liquids
journal, July 2008

Pressure and temperature dependence of structural relaxation in diglycidylether of bisphenol A
journal, February 2003

Correlation of fragility of supercooled liquids with elastic properties of glasses
journal, June 2005

Stokes–Einstein relation in dense metallic glass-forming melts
journal, November 2010

Little evidence for dynamic divergences in ultraviscous molecular liquids
journal, July 2008

Kinetic fragility of Se-based binary chalcogenide glasses
journal, July 2015

Comment on “High-Frequency Dynamics in Metallic Glasses”
journal, February 2007

Theory of non-linear susceptibility and correlation length in glasses and liquids
journal, September 2002

Supercooled liquids and the glass transition
journal, March 2001

Dynamics and energy landscape in a tetrahedral network glass-former: direct comparison with models of fragile liquids
journal, June 2009

Heterogeneous dynamics in liquids: fluctuations in space and time
journal, May 2002

High-Frequency Dynamics in Metallic Glasses
journal, April 2006

Poisson's ratio and the fragility of glass-forming liquids
journal, October 2004

Atomic transport in dense multicomponent metallic liquids
journal, October 2002

Two-step relaxation in a viscous metallic liquid
journal, August 1999

Characteristic relaxation times and their invariance to thermodynamic conditions
journal, January 2008

Proposal for universality in the viscosity of metallic liquids
journal, September 2015

Theory of dynamic barriers, activated hopping, and the glass transition in polymer melts
journal, July 2004

A macroscopic model that connects the molar excess entropy of a supercooled liquid near its glass transition temperature to its viscosity
journal, November 2012

Universality of the dynamic crossover in glass-forming liquids: A “magic” relaxation time
journal, March 2003

Atomic dynamics in binary Zr-Cu liquids
journal, August 2014

Obtaining the glass transition temperature by measuring the crack healing process of glassformers
journal, March 2008

Correlation between fragility and cooperativity in bulk metallic glass-forming liquids
journal, October 2010

Temperature Dependence of the Segmental Relaxation Time of Polymers Revisited
journal, April 2015

Fast and slow dynamics in Pr60Ni10Cu20Al10 melts as seen by neutron scattering
journal, January 2008

Dynamic fragility in polymers: A comparison in isobaric and isochoric conditions
journal, March 2002

Viscosity of titania-bearing sodium silicate melts
journal, June 1996

Universal representation of viscosity in glass forming liquids
journal, January 1998

Formation of Glasses from Liquids and Biopolymers
journal, March 1995

Elastically cooperative activated barrier hopping theory of relaxation in viscous fluids. II. Thermal liquids
journal, May 2014