Microscopic Theory for the Role of Attractive Forces in the Dynamics of Supercooled Liquids

Dell, Zachary E.; Schweizer, Kenneth S.

doi:10.1103/physrevlett.115.205702

Title: Microscopic Theory for the Role of Attractive Forces in the Dynamics of Supercooled Liquids

Journal Article · 10 November 2015 · Physical Review Letters

DOI: https://doi.org/10.1103/physrevlett.115.205702 · OSTI ID:1875671

Dell, Zachary E. ^[1]; Schweizer, Kenneth S. ^[2]

Univ. of Illinois, Urbana, IL (United States); University of Illinois
Univ. of Illinois, Urbana, IL (United States)

We formulate a microscopic, no adjustable parameter, theory of activated relaxation in supercooled liquids directly in terms of the repulsive and attractive forces within the framework of pair correlations. Under isochoric conditions, attractive forces can nonperturbatively modify slow dynamics, but at high enough density their influence vanishes. Under isobaric conditions, attractive forces play a minor role. High temperature apparent Arrhenius behavior and density-temperature scaling are predicted. Furthermore, our results are consistent with recent isochoric simulations and isobaric experiments on a deeply supercooled molecular liquid. The approach can be generalized to treat colloidal gelation and glass melting, and other soft matter slow dynamics problems.

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Research Organization:: Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-07ER46471

OSTI ID:: 1875671

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 20 Vol. 115; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (48)

Determination of Lennard-Jones interaction parameters using a new procedure Cuadros, F.; Cachadiña, I.; Ahumada, W. Molecular Engineering, Vol. 6, Issue 3 https://doi.org/10.1007/BF01886380	journal	September 1996
Indications for a change of transport mechanism in supercooled liquids and the dynamics close and below Tg Rössler, E.; Warschewske, U.; Eiermann, P. Journal of Non-Crystalline Solids, Vol. 172-174 https://doi.org/10.1016/0022-3093(94)90424-3	journal	September 1994
Source of non-Arrhenius average relaxation time in glass-forming liquids Dyre, Jeppe C. Journal of Non-Crystalline Solids, Vol. 235-237 https://doi.org/10.1016/S0022-3093(98)00502-X	journal	August 1998
Isobaric and isochoric properties of decahydroisoquinoline, an extremely fragile glass-former Casalini, R.; McGrath, K. J.; Roland, C. M. Journal of Non-Crystalline Solids, Vol. 352, Issue 42-49 https://doi.org/10.1016/j.jnoncrysol.2006.02.151	journal	November 2006
Supercooled liquids for pedestrians Cavagna, Andrea Physics Reports, Vol. 476, Issue 4-6 https://doi.org/10.1016/j.physrep.2009.03.003	journal	June 2009
Intermolecular forces in biology Leckband, Deborah; Israelachvili, Jacob Quarterly Reviews of Biophysics, Vol. 34, Issue 2 https://doi.org/10.1017/S0033583501003687	journal	May 2001
Comparison of Dynamical Heterogeneity in Hard-Sphere and Attractive Glass Formers ^† Reichman, David R.; Rabani, Eran; Geissler, Phillip L. The Journal of Physical Chemistry B, Vol. 109, Issue 30 https://doi.org/10.1021/jp044559n	journal	August 2005
Corresponding States of Structural Glass Formers. II Elmatad, Yael S.; Chandler, David; Garrahan, Juan P. The Journal of Physical Chemistry B, Vol. 114, Issue 51 https://doi.org/10.1021/jp1076438	journal	December 2010
Hidden Scale Invariance in Condensed Matter Dyre, Jeppe C. The Journal of Physical Chemistry B, Vol. 118, Issue 34 https://doi.org/10.1021/jp501852b	journal	July 2014
Unified Theory of Activated Relaxation in Liquids over 14 Decades in Time Mirigian, Stephen; Schweizer, Kenneth S. The Journal of Physical Chemistry Letters, Vol. 4, Issue 21 https://doi.org/10.1021/jz4018943	journal	October 2013
Dynamical Theory of Segmental Relaxation and Emergent Elasticity in Supercooled Polymer Melts Mirigian, Stephen; Schweizer, Kenneth S. Macromolecules, Vol. 48, Issue 6 https://doi.org/10.1021/ma5022083	journal	March 2015
Equation of State for Lennard-Jones Fluid Boltachev, G. Sh. High Temperature, Vol. 41, Issue 2, p. 270-272 https://doi.org/10.1023/A:1023394122000	journal	March 2003
One liquid, two glasses Sciortino, Francesco Nature Materials, Vol. 1, Issue 3 https://doi.org/10.1038/nmat752	journal	November 2002
Role of Repulsive Forces in Determining the Equilibrium Structure of Simple Liquids Weeks, John D.; Chandler, David; Andersen, Hans C. The Journal of Chemical Physics, Vol. 54, Issue 12 https://doi.org/10.1063/1.1674820	journal	June 1971
Perturbation Theory and Equation of State for Fluids. II. A Successful Theory of Liquids Barker, J. A.; Henderson, D. The Journal of Chemical Physics, Vol. 47, Issue 11 https://doi.org/10.1063/1.1701689	journal	December 1967
Derivation of a microscopic theory of barriers and activated hopping transport in glassy liquids and suspensions Schweizer, Kenneth S. The Journal of Chemical Physics, Vol. 123, Issue 24 https://doi.org/10.1063/1.2137701	journal	December 2005
Activated hopping and dynamical fluctuation effects in hard sphere suspensions and fluids Saltzman, Erica J.; Schweizer, Kenneth S. The Journal of Chemical Physics, Vol. 125, Issue 4 https://doi.org/10.1063/1.2217739	journal	July 2006
Direct imaging of repulsive and attractive colloidal glasses Kaufman, Laura J.; Weitz, David A. The Journal of Chemical Physics, Vol. 125, Issue 7 https://doi.org/10.1063/1.2227386	journal	August 2006
Collisions, caging, thermodynamics, and jamming in the barrier hopping theory of glassy hard sphere fluids Schweizer, Kenneth S.; Yatsenko, Galina The Journal of Chemical Physics, Vol. 127, Issue 16 https://doi.org/10.1063/1.2780861	journal	October 2007
The influence of shape on the glassy dynamics of hard nonspherical particle fluids. I. Dynamic crossover and elasticity Tripathy, Mukta; Schweizer, Kenneth S. The Journal of Chemical Physics, Vol. 130, Issue 24 https://doi.org/10.1063/1.3157279	journal	June 2009
Glassy dynamics and mechanical response in dense fluids of soft repulsive spheres. I. Activated relaxation, kinetic vitrification, and fragility Yang, Jian; Schweizer, Kenneth S. The Journal of Chemical Physics, Vol. 134, Issue 20 https://doi.org/10.1063/1.3592563	journal	May 2011
The role of attractive forces in viscous liquids Berthier, Ludovic; Tarjus, Gilles The Journal of Chemical Physics, Vol. 134, Issue 21 https://doi.org/10.1063/1.3592709	journal	June 2011
Vibrational dephasing and frequency shifts of polyatomic molecules in solution Schweizer, Kenneth S.; Chandler, David The Journal of Chemical Physics, Vol. 76, Issue 5 https://doi.org/10.1063/1.443302	journal	March 1982
Microscopic theory of the dynamics of polymeric liquids: General formulation of a mode–mode‐coupling approach Schweizer, Kenneth S. The Journal of Chemical Physics, Vol. 91, Issue 9 https://doi.org/10.1063/1.457533	journal	November 1989
Static triplet correlations in glass-forming liquids: A molecular dynamics study Coslovich, Daniele The Journal of Chemical Physics, Vol. 138, Issue 12 https://doi.org/10.1063/1.4773355	journal	March 2013
Effect of chain flexibility on master curve behavior for diffusion coefficient Budzien, Joanne; Heffernan, Julieanne V.; McCoy, John D. The Journal of Chemical Physics, Vol. 139, Issue 24 https://doi.org/10.1063/1.4851437	journal	December 2013
Elastically cooperative activated barrier hopping theory of relaxation in viscous fluids. I. General formulation and application to hard sphere fluids Mirigian, Stephen; Schweizer, Kenneth S. The Journal of Chemical Physics, Vol. 140, Issue 19 https://doi.org/10.1063/1.4874842	journal	May 2014
Elastically cooperative activated barrier hopping theory of relaxation in viscous fluids. II. Thermal liquids Mirigian, Stephen; Schweizer, Kenneth S. The Journal of Chemical Physics, Vol. 140, Issue 19 https://doi.org/10.1063/1.4874843	journal	May 2014
Supercooled dynamics of glass-forming liquids and polymers under hydrostatic pressure Roland, C. M.; Hensel-Bielowka, S.; Paluch, M. Reports on Progress in Physics, Vol. 68, Issue 6 https://doi.org/10.1088/0034-4885/68/6/R03	journal	May 2005
Colloidal gels: equilibrium and non-equilibrium routes Zaccarelli, Emanuela Journal of Physics: Condensed Matter, Vol. 19, Issue 32 https://doi.org/10.1088/0953-8984/19/32/323101	journal	July 2007
Do the repulsive and attractive pair forces play separate roles for the physics of liquids? Bøhling, Lasse; Veldhorst, Arno A.; Ingebrigtsen, Trond S. Journal of Physics: Condensed Matter, Vol. 25, Issue 3 https://doi.org/10.1088/0953-8984/25/3/032101	journal	December 2012
Connections between some kinetic and equilibrium theories of the glass transition Kirkpatrick, T. R.; Wolynes, P. G. Physical Review A, Vol. 35, Issue 7 https://doi.org/10.1103/PhysRevA.35.3072	journal	April 1987
Nonergodicity transitions in colloidal suspensions with attractive interactions Bergenholtz, J.; Fuchs, M. Physical Review E, Vol. 59, Issue 5 https://doi.org/10.1103/PhysRevE.59.5706	journal	May 1999
Theory of coupled translational-rotational glassy dynamics in dense fluids of uniaxial particles Zhang, Rui; Schweizer, Kenneth S. Physical Review E, Vol. 80, Issue 1 https://doi.org/10.1103/PhysRevE.80.011502	journal	July 2009
Critical test of the mode-coupling theory of the glass transition Berthier, Ludovic; Tarjus, Gilles Physical Review E, Vol. 82, Issue 3 https://doi.org/10.1103/PhysRevE.82.031502	journal	September 2010
Activated dynamics in dense fluids of attractive nonspherical particles. I. Kinetic crossover, dynamic free energies, and the physical nature of glasses and gels Tripathy, Mukta; Schweizer, Kenneth S. Physical Review E, Vol. 83, Issue 4 https://doi.org/10.1103/PhysRevE.83.041406	journal	April 2011
Kinetic arrest, dynamical transitions, and activated relaxation in dense fluids of attractive nonspherical colloids Zhang, Rui; Schweizer, Kenneth S. Physical Review E, Vol. 83, Issue 6 https://doi.org/10.1103/PhysRevE.83.060502	journal	June 2011
Probing the Equilibrium Dynamics of Colloidal Hard Spheres above the Mode-Coupling Glass Transition Brambilla, G.; El Masri, D.; Pierno, M. Physical Review Letters, Vol. 102, Issue 8 https://doi.org/10.1103/PhysRevLett.102.085703	journal	February 2009
Nonperturbative Effect of Attractive Forces in Viscous Liquids Berthier, Ludovic; Tarjus, Gilles Physical Review Letters, Vol. 103, Issue 17 https://doi.org/10.1103/PhysRevLett.103.170601	journal	October 2009
Repulsive Reference Potential Reproducing the Dynamics of a Liquid with Attractions Pedersen, Ulf R.; Schrøder, Thomas B.; Dyre, Jeppe C. Physical Review Letters, Vol. 105, Issue 15 https://doi.org/10.1103/PhysRevLett.105.157801	journal	October 2010
Growing Point-to-Set Length Scale Correlates with Growing Relaxation Times in Model Supercooled Liquids Hocky, Glen M.; Markland, Thomas E.; Reichman, David R. Physical Review Letters, Vol. 108, Issue 22 https://doi.org/10.1103/PhysRevLett.108.225506	journal	June 2012
Comparative Simulation Study of Colloidal Gels And Glasses Puertas, Antonio M.; Fuchs, Matthias; Cates, Michael E. Physical Review Letters, Vol. 88, Issue 9 https://doi.org/10.1103/PhysRevLett.88.098301	journal	February 2002
Colloquium : The glass transition and elastic models of glass-forming liquids Dyre, Jeppe C. Reviews of Modern Physics, Vol. 78, Issue 3 https://doi.org/10.1103/RevModPhys.78.953	journal	September 2006
Theoretical perspective on the glass transition and amorphous materials Berthier, Ludovic; Biroli, Giulio Reviews of Modern Physics, Vol. 83, Issue 2 https://doi.org/10.1103/RevModPhys.83.587	journal	June 2011
Multiple Glassy States in a Simple Model System Pham, K. N. Science, Vol. 296, Issue 5565 https://doi.org/10.1126/science.1068238	journal	April 2002
Intermolecular Forces and the Nature of the Liquid State: Liquids reflect in their bulk properties the attractions and repulsions of their constituent molecules Widom, B. Science, Vol. 157, Issue 3787 https://doi.org/10.1126/science.157.3787.375	journal	July 1967
Testing “microscopic” theories of glass-forming liquids Berthier, L.; Tarjus, G. The European Physical Journal E, Vol. 34, Issue 9 https://doi.org/10.1140/epje/i2011-11096-5	journal	September 2011
Tunable dynamic fragility and elasticity in dense suspensions of many-arm-star polymer colloids Yang, Jian; S. Schweizer, Kenneth EPL (Europhysics Letters), Vol. 90, Issue 6 https://doi.org/10.1209/0295-5075/90/66001	journal	June 2010

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