Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy

Zhang, Pei; Maldonis, Jason J.; Liu, Ze; Schroers, Jan; Voyles, Paul M.

doi:10.1038/s41467-018-03604-2

Title: Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy

Abstract

Supercooled liquids exhibit spatial heterogeneity in the dynamics of their fluctuating atomic arrangements. The length and time scales of the heterogeneous dynamics are central to the glass transition and influence nucleation and growth of crystals from the liquid. In this work, we report direct experimental visualization of the spatially heterogeneous dynamics as a function of temperature in the supercooled liquid state of a Pt-based metallic glass, using electron correlation microscopy with sub-nanometer resolution. An experimental four-point space-time correlation function demonstrates a growing dynamic correlation length, ξ, upon cooling of the liquid toward the glass transition temperature. ξ as a function of the relaxation time τ are in good agreement with Adam-Gibbs theory, inhomogeneous mode-coupling theory and random first-order transition theory of the glass transition. The same experiments demonstrate the existence of a nanometer thickness near-surface layer with order of magnitude shorter relaxation time than inside the bulk.

Authors:

Zhang, Pei ^[1];

^[1]; Liu, Ze ^[2]; Schroers, Jan ^[2];

^[1]

Univ. of Wisconsin, Madison, WI (United States)
Yale Univ., New Haven, CT (United States)

Publication Date:: 2018-03-19

Research Org.:: Yale Univ., New Haven, CT (United States)

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

OSTI Identifier:: 1526297

Grant/Contract Number:: SC0004889; DMR-1121288; DMR-1506564

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 42 ENGINEERING

Citation Formats


                    Zhang, Pei, Maldonis, Jason J., Liu, Ze, Schroers, Jan, and Voyles, Paul M. Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy.  United States: N. p., 2018. 
Web.  doi:10.1038/s41467-018-03604-2.

Copy to clipboard


                    Zhang, Pei, Maldonis, Jason J., Liu, Ze, Schroers, Jan, & Voyles, Paul M. Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy.  United States.  https://doi.org/10.1038/s41467-018-03604-2

Copy to clipboard


                    Zhang, Pei, Maldonis, Jason J., Liu, Ze, Schroers, Jan, and Voyles, Paul M. Mon .  
"Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy".  United States.  https://doi.org/10.1038/s41467-018-03604-2.  https://www.osti.gov/servlets/purl/1526297.

Copy to clipboard


                    
@article{osti_1526297,

  title        = {Spatially heterogeneous dynamics in a metallic glass forming liquid imaged by electron correlation microscopy},

  author       = {Zhang, Pei and Maldonis, Jason J. and Liu, Ze and Schroers, Jan and Voyles, Paul M.},

  abstractNote = {Supercooled liquids exhibit spatial heterogeneity in the dynamics of their fluctuating atomic arrangements. The length and time scales of the heterogeneous dynamics are central to the glass transition and influence nucleation and growth of crystals from the liquid. In this work, we report direct experimental visualization of the spatially heterogeneous dynamics as a function of temperature in the supercooled liquid state of a Pt-based metallic glass, using electron correlation microscopy with sub-nanometer resolution. An experimental four-point space-time correlation function demonstrates a growing dynamic correlation length, ξ, upon cooling of the liquid toward the glass transition temperature. ξ as a function of the relaxation time τ are in good agreement with Adam-Gibbs theory, inhomogeneous mode-coupling theory and random first-order transition theory of the glass transition. The same experiments demonstrate the existence of a nanometer thickness near-surface layer with order of magnitude shorter relaxation time than inside the bulk.},

  doi          = {10.1038/s41467-018-03604-2},

  journal      = {Nature Communications},

  number       = 1,

  volume       = 9,

  place        = {United States},

  year         = {2018},

  month        = {3}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

https://doi.org/10.1038/s41467-018-03604-2

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 18 works

Citation information provided by
Web of Science

Figures / Tables:

Fig. 1: Tilted dark-field electron correlation microscopy. a Schematic of the experiment. Tilted illumination shifts the transmitted beam off the optic axis of a microscope. A small, on-axis objective aperture selects one speckle in the diffraction pattern, forming a real-space image. Structural rearrangements cause fluctuations in the intensity of themore »

All figures and tables (4 total)

Save / Share:

Export Metadata

Save to My Library

Works referenced in this record:

Growing length and time scales in glass-forming liquids
journal, February 2009

Karmakar, S.; Dasgupta, C.; Sastry, S.
Proceedings of the National Academy of Sciences, Vol. 106, Issue 10
DOI: 10.1073/pnas.0811082106

Correlation spectroscopy with coherent X-rays
journal, January 2004

Grübel, Gerhard; Zontone, Federico
Journal of Alloys and Compounds, Vol. 362, Issue 1-2
DOI: 10.1016/S0925-8388(03)00555-3

Dynamical Heterogeneities in a Supercooled Lennard-Jones Liquid
journal, October 1997

Kob, Walter; Donati, Claudio; Plimpton, Steven J.
Physical Review Letters, Vol. 79, Issue 15
DOI: 10.1103/PhysRevLett.79.2827

Spatially heterogeneous dynamics investigated via a time-dependent four-point density correlation function
journal, October 2003

Lačević, N.; Starr, F. W.; Schrøder, T. B.
The Journal of Chemical Physics, Vol. 119, Issue 14
DOI: 10.1063/1.1605094

Dynamics of highly supercooled liquids: Heterogeneity, rheology, and diffusion
journal, September 1998

Yamamoto, Ryoichi; Onuki, Akira
Physical Review E, Vol. 58, Issue 3
DOI: 10.1103/PhysRevE.58.3515

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

Berthier, Ludovic; Biroli, Giulio
Reviews of Modern Physics, Vol. 83, Issue 2
DOI: 10.1103/RevModPhys.83.587

Atomic-Scale Relaxation Dynamics and Aging in a Metallic Glass Probed by X-Ray Photon Correlation Spectroscopy
journal, October 2012

Ruta, B.; Chushkin, Y.; Monaco, G.
Physical Review Letters, Vol. 109, Issue 16
DOI: 10.1103/PhysRevLett.109.165701

When the Heterogeneous Appears Homogeneous: Discrepant Measures of Heterogeneity in Single-Molecule Observables
journal, February 2011

Mackowiak, Stephan A.; Kaufman, Laura J.
The Journal of Physical Chemistry Letters, Vol. 2, Issue 5
DOI: 10.1021/jz1016872

Fast Surface Diffusion of Amorphous o -Terphenyl and Its Competition with Viscous Flow in Surface Evolution
journal, April 2015

Zhang, Wei; Brian, Caleb W.; Yu, Lian
The Journal of Physical Chemistry B, Vol. 119, Issue 15
DOI: 10.1021/jp5127464

Dielectric beta relaxations in the glassy state of salol?
journal, June 1999

Wagner, Hermann; Richert, Ranko
The Journal of Chemical Physics, Vol. 110, Issue 23
DOI: 10.1063/1.479105

Thermodynamics, kinetics, and crystallization of Pt57.3Cu14.6Ni5.3P22.8 bulk metallic glass
journal, February 2007

Legg, Benjamin A.; Schroers, Jan; Busch, Ralf
Acta Materialia, Vol. 55, Issue 3
DOI: 10.1016/j.actamat.2006.09.024

Viscoelasticity and viscosity of Pd–Ni–Cu–P bulk metallic glasses
journal, October 2002

Pelletier, J. M.; Van de Moortèle, B.; Lu, I. R.
Materials Science and Engineering: A, Vol. 336, Issue 1-2
DOI: 10.1016/S0921-5093(01)01967-0

Slow relaxations in deeply undercooled metallic liquids
journal, October 2002

Wilde, Gerhard
Journal of Non-Crystalline Solids, Vol. 312-314
DOI: 10.1016/S0022-3093(02)01753-2

Dynamical susceptibility of glass formers: Contrasting the predictions of theoretical scenarios
journal, April 2005

Toninelli, Cristina; Wyart, Matthieu; Berthier, Ludovic
Physical Review E, Vol. 71, Issue 4
DOI: 10.1103/PhysRevE.71.041505

Time‐dependent correlation and the evaluation of the stretched exponential or Kohlrausch–Williams–Watts function
journal, November 1991

Chung, S. H.; Stevens, J. R.
American Journal of Physics, Vol. 59, Issue 11
DOI: 10.1119/1.16640

Three-Dimensional Direct Imaging of Structural Relaxation Near the Colloidal Glass Transition
journal, January 2000

Weeks, E. R.
Science, Vol. 287, Issue 5453
DOI: 10.1126/science.287.5453.627

On the Temperature Dependence of Cooperative Relaxation Properties in Glass‐Forming Liquids
journal, July 1965

Adam, Gerold; Gibbs, Julian H.
The Journal of Chemical Physics, Vol. 43, Issue 1
DOI: 10.1063/1.1696442

Testing mode-coupling theory for a supercooled binary Lennard-Jones mixture. II. Intermediate scattering function and dynamic susceptibility
journal, October 1995

Kob, Walter; Andersen, Hans C.
Physical Review E, Vol. 52, Issue 4
DOI: 10.1103/PhysRevE.52.4134

Real-Space Imaging of Nucleation and Growth in Colloidal Crystallization
journal, April 2001

Gasser, U.
Science, Vol. 292, Issue 5515
DOI: 10.1126/science.1058457

Comparison of fluctuation electron microscopy theories and experimental methods
journal, October 2007

Stratton, W. G.; Voyles, P. M.
Journal of Physics: Condensed Matter, Vol. 19, Issue 45
DOI: 10.1088/0953-8984/19/45/455203

Inhomogeneous Mode-Coupling Theory and Growing Dynamic Length in Supercooled Liquids
journal, November 2006

Biroli, Giulio; Bouchaud, Jean-Philippe; Miyazaki, Kunimasa
Physical Review Letters, Vol. 97, Issue 19
DOI: 10.1103/PhysRevLett.97.195701

High surface mobility and fast surface enhanced crystallization of metallic glass
journal, October 2015

Cao, C. R.; Lu, Y. M.; Bai, H. Y.
Applied Physics Letters, Vol. 107, Issue 14
DOI: 10.1063/1.4933036

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

Keys, Aaron S.; Abate, Adam R.; Glotzer, Sharon C.
Nature Physics, Vol. 3, Issue 4
DOI: 10.1038/nphys572

Crystal nucleation in deeply undercooled melts of bulk metallic glass forming systems
journal, January 2002

Assadi, Hamid; Schroers, Jan
Acta Materialia, Vol. 50, Issue 1
DOI: 10.1016/S1359-6454(01)00319-6

The dynamics of the spreading of liquids on a solid surface. Part 1. Viscous flow
journal, July 1986

Cox, R. G.
Journal of Fluid Mechanics, Vol. 168, Issue -1
DOI: 10.1017/S0022112086000332

Nanomoulding with amorphous metals
journal, February 2009

Kumar, Golden; Tang, Hong X.; Schroers, Jan
Nature, Vol. 457, Issue 7231
DOI: 10.1038/nature07718

Light-scattering investigation of α and β relaxation near the liquid-glass transition of the molecular glass Salol
journal, September 1992

Li, G.; Du, W. M.; Sakai, A.
Physical Review A, Vol. 46, Issue 6
DOI: 10.1103/PhysRevA.46.3343

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

Richert, Ranko
Journal of Physics: Condensed Matter, Vol. 14, Issue 23
DOI: 10.1088/0953-8984/14/23/201

Activation energy for surface diffusion of Si on Si(001): A scanning-tunneling-microscopy study
journal, April 1991

Mo, Y. W.; Kleiner, J.; Webb, M. B.
Physical Review Letters, Vol. 66, Issue 15
DOI: 10.1103/PhysRevLett.66.1998

Effect of finite trajectory length on the correlation function analysis of single molecule data
journal, September 2006

Lu, Chun-Yaung; Vanden Bout, David A.
The Journal of Chemical Physics, Vol. 125, Issue 12
DOI: 10.1063/1.2352748

Electron Correlation Microscopy: A New Technique for Studying Local Atom Dynamics Applied to a Supercooled Liquid
journal, June 2015

He, Li; Zhang, Pei; Besser, Matthew F.
Microscopy and Microanalysis, Vol. 21, Issue 4
DOI: 10.1017/S1431927615000641

Fifth-order susceptibility unveils growth of thermodynamic amorphous order in glass-formers
journal, June 2016

Albert, S.; Bauer, T.; Michl, M.
Science, Vol. 352, Issue 6291
DOI: 10.1126/science.aaf3182

Giant fluctuations in a free diffusion process
journal, November 1997

Vailati, Alberto; Giglio, Marzio
Nature, Vol. 390, Issue 6657
DOI: 10.1038/36803

Time-dependent, four-point density correlation function description of dynamical heterogeneity and decoupling in supercooled liquids
journal, January 2000

Glotzer, Sharon C.; Novikov, Vladimir N.; Schrøder, Thomas B.
The Journal of Chemical Physics, Vol. 112, Issue 2
DOI: 10.1063/1.480541

Cooperative strings and glassy interfaces
journal, June 2015

Salez, Thomas; Salez, Justin; Dalnoki-Veress, Kari
Proceedings of the National Academy of Sciences, Vol. 112, Issue 27
DOI: 10.1073/pnas.1503133112

On the diffuse interface theory of nucleation
journal, March 1994

Gránásy, L.; Egry, I.; Ratke, L.
Scripta Metallurgica et Materialia, Vol. 30, Issue 5
DOI: 10.1016/0956-716X(94)90440-5

Note: Effects of adding a viscosity-increasing 2 nm-size molecule on dielectric relaxation features and the dynamic heterogeneity view
journal, May 2013

Khouri, Joseph; Johari, G. P.
The Journal of Chemical Physics, Vol. 138, Issue 19
DOI: 10.1063/1.4807006

Non-exponentiality of structural relaxations in glass forming metallic liquids
journal, August 2010

Wang, Li-Min; Chen, Zeming; Zhao, Yue
Journal of Alloys and Compounds, Vol. 504
DOI: 10.1016/j.jallcom.2010.04.011