TY - JOUR
T1 - Energy Renormalization for Coarse-Graining the Dynamics of a Model Glass-Forming Liquid
AU - Xia, Wenjie
AU - Song, Jake
AU - Hansoge, Nitin K.
AU - Phelan, Frederick R.
AU - Keten, Sinan
AU - Douglas, Jack F.
N1 - Funding Information:
The authors acknowledge support by the National Institute of Standards and Technology (NIST) through the Center for Hierarchical Materials Design (CHiMaD). W.X., J.S., N.K.H., and S.K. acknowledge support from the Department of Civil & Environmental Engineering, Mechanical Engineering and Materials Science and Engineering at Northwestern University. W.X. gratefully acknowledges the support from the NIST-CHiMaD Postdoctoral Fellowship. S.K. acknowledges the support from an ONR Director of Research Early Career Award (PECASE, award #N00014163175). Supercomputing grants from the Raritan HPC System at NIST and the Quest HPC System at Northwestern University are acknowledged.
Publisher Copyright:
© 2018 American Chemical Society.
PY - 2018/2/15
Y1 - 2018/2/15
N2 - Coarse-grained modeling achieves the enhanced computational efficiency required to model glass-forming materials by integrating out "unessential" molecular degrees of freedom, but no effective temperature transferable coarse-graining method currently exists to capture dynamics. We address this fundamental problem through an energy-renormalization scheme, in conjunction with the localization model of relaxation relating the Debye-Waller factor «u2» to the structural relaxation time τ. Taking ortho-terphenyl as a model small-molecule glass-forming liquid, we show that preserving «u2» (at picosecond time scale) under coarse-graining by renormalizing the cohesive interaction strength allows for quantitative prediction of both short- and long-time dynamics covering the entire temperature range of glass formation. Our findings provide physical insights into the dynamics of cooled liquids and make progress for building temperature-transferable coarse-grained models that predict key properties of glass-forming materials.
AB - Coarse-grained modeling achieves the enhanced computational efficiency required to model glass-forming materials by integrating out "unessential" molecular degrees of freedom, but no effective temperature transferable coarse-graining method currently exists to capture dynamics. We address this fundamental problem through an energy-renormalization scheme, in conjunction with the localization model of relaxation relating the Debye-Waller factor «u2» to the structural relaxation time τ. Taking ortho-terphenyl as a model small-molecule glass-forming liquid, we show that preserving «u2» (at picosecond time scale) under coarse-graining by renormalizing the cohesive interaction strength allows for quantitative prediction of both short- and long-time dynamics covering the entire temperature range of glass formation. Our findings provide physical insights into the dynamics of cooled liquids and make progress for building temperature-transferable coarse-grained models that predict key properties of glass-forming materials.
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U2 - 10.1021/acs.jpcb.8b00321
DO - 10.1021/acs.jpcb.8b00321
M3 - Article
C2 - 29400063
AN - SCOPUS:85042169215
SN - 1520-6106
VL - 122
SP - 2040
EP - 2045
JO - Journal of Physical Chemistry B
JF - Journal of Physical Chemistry B
IS - 6
ER -