Abstract
Coupled length and time scales determine the dynamic behavior of polymers and polymer nanocomposites, thus causing their unique properties. To resolve the properties over large time and length scales it is imperative to develop coarse-grained models which retain atomistic specificity. Here we probe the degree of coarse graining required to access large length and time scales and simultaneously retain significant atomistic details. The degree of coarse graining in turn sets the minimum length scale instrumental in defining polymer properties and dynamics. Using polyethylene as a model system, we probe how the scale of coarse graining affects the measured dynamics with different number of methylene groups per coarse-grained bead. Using these models, it is currently possible to simulate polyethylene melts for times of order 1 millisecond. This allows one to study a wide range of properties from chain mobility to viscoelastic response for well-entangled polymer melts while retaining atomistic detail.
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Abrams CF, Kremer K (2003) Combined coarse-grained and atomistic simulation of liquid bisphenol a−polycarbonate: liquid packing and intramolecular structure. Macromolecules 36:260–267
Ashbaugh HS, Patel HA, Kumar SK, Garde S (2005) Mesoscale model of polymer melt structure: self-consistent mapping of molecular correlations to coarse-grained potentials. J Chem Phys 122:104908
Chen L-J, Qian H-J, Lu Z-Y, Li Z-S, Sun C-C (2006) An automatic coarse-graining and fine-graining simulation method: application on polyethylene. J Phys Chem B 110:24093–24100
Curcó D, Alemán C (2007) Coarse-grained simulations of amorphous and melted polyethylene. Chem Phys Lett 436:189–193
Dallavalle M, van der Vegt NFA (2017) Evaluation of mapping schemes for systematic coarse graining of higher alkanes. Phys Chem Chem Phys 19:23034–23042
Doi M, Edwards SF (1986) The theory of polymer dynamics. Oxford University, Oxford, UK
Everaers R, Sukumaran SK, Grest GS, Svaneborg C, Sivasubramanian A, Kremer K (2004) Rheology and microscopic topology of entangled polymeric liquids. Science 303:823–826
Ferry JD (1980) Viscoelastic properties of polymers. Wiley, New York
Fetters LJ, Lohse DJ, Milner ST, Graessley WW (1999) Packing length influence in linear polymer melts on the entanglement, critical, and reptation molecular weights. Macromolecules 32:6847–6851
Fritz D, Koschke K, Harmandaris VA, van der Vegt NF, Kremer K (2011) Multiscale modeling of soft matter: scaling of dynamics. Phys Chem Chem Phys 13:10412–10420
Fukunaga H, Takimoto J-i, Doi M (2002) A coarse-graining procedure for flexible polymer chains with bonded and nonbonded interactions. J Chem Phys 116:8183–8190
de Gennes P-G (1971) Reptation of a polymer chain in the presence of fixed obstacles. J Chem Phys 55:572–579
Graessley WW, Edwards SF (1981) Entanglement interactions in polymers and the chain contour concentration. Polymer 22:1329–1334
Grest GS (2016) Communication: polymer entanglement dynamics: role of attractive interactions. J Chem Phys 145:141101
Guerrault X, Rousseau B, Farago J (2004) Dissipative particle dynamics simulations of polymer melts. I. Building potential of mean force for polyethylene and cis-polybutadiene. J Chem Phys 121:6538–6546
Harmandaris VA, Kremer K (2009) Dynamics of polystyrene melts through hierarchical multiscale simulations. Macromolecules 42:791–802
Harmandaris VA, Reith D, van der Vegt NFA, Kremer K (2007) Comparison between coarse-graining models for polymer systems: two mapping schemes for polystyrene. Macromol Chem Phys 208:2109–2120
Hou J-X (2017) Note: determine entanglement length through monomer mean-square displacement. J Chem Phys 146:026101
Hoy RS, Grest GS (2007) Entanglements of an end-grafted polymer brush in a polymeric matrix. Macromolecules 40:8389–8395
Hoy RS, Foteinopoulou K, Kröger M (2009) Topological analysis of polymeric melts: chain-length effects and fast-converging estimators for entanglement length. Phys Rev E 80:031803
Hsu H-P, Kremer K (2016) Static and dynamic properties of large polymer melts in equilibrium. J Chem Phys 144:154907
Hsu H-P, Kremer K (2017) Detailed analysis of Rouse mode and dynamic scattering function of highly entangled polymer melts in equilibrium. Euro Phys J Special Topics 226:693–703
Jorgensen WL, Madura JD, Swenson CJ (1984) Optimized intermolecular potential functions for liquid hydrocarbons. J Am Chem Soc 106:6638–6646
Jorgensen WL, Maxwell DS, Tirado-Rives J (1996) Development and testing of the OPLS all-atom force field on conformational energetics and properties of organic liquids. J Am Chem Soc 118(45):11225–11236
Karimi-Varzabeh HA, van der Vegt NFA, Mueller-Plathe F, Carbone P (2012) How good are coarse-grained models? A comparison for actatic polystyrene. ChemPhysChem 13:3428–3439
Kremer K, Grest GS (1990) Dynamics of entangled linear polymer melts: a molecular-dynamics simulation. J Chem Phys 92:5057–5086
Li Y, Abberton BC, Kröger M, Liu WK (2013) Challenges in multiscale modeling of polymer dynamics. Polymer 5:751–832
Likhtman AE, McLeish TC (2002) Quantitative theory for linear dynamics of linear entangled polymers. Macromolecules 35:6332–6343
Lodge TP (1999) Reconciliation of the molecular weight dependence of diffusion and viscosity in entangled polymers. Phys Rev Lett 83:3218
Marrucci G (1985) Relaxation by reptation and tube enlargement: a model for polydisperse polymers. J Polym Sci B Polym Phys 23:159–177
Martin MG, Siepmann JI (1998) Transferable potentials for phase equilibria. 1. United-atom description of n-alkanes. J Phys Chem B 102:2569–2577
Maurel G, Schnell B, Goujon F, Couty M, Malfreyt P (2012) Multiscale modeling approach toward the prediction of viscoelastic properties of polymers. J Chem Theory Comput 8:4570–4579
Maurel G, Goujon F, Schnell B, Malfreyt P (2015) Prediction of structural and thermomechanical properties of polymers from multiscale simulations. RSC Adv 5(19):14065–14073
Milano G, Müller-Plathe F (2005) Mapping atomistic simulations to mesoscopic models: a systematic coarse-graining procedure for vinyl polymer chains. J Phys Chem B 109:18609–18619
Müller-Plathe F (2002) Coarse-graining in polymer simulation: from the atomistic to the mesoscopic scale and back. ChemPhysChem 3:754–769
Nath SK, Escobedo FA, de Pablo JJ (1998) On the simulation of vapor–liquid equilibria for alkanes. J Chem Phys 108:9905–9911
Padding J, Briels WJ (2001) Uncrossability constraints in mesoscopic polymer melt simulations: non-Rouse behavior of CH. J Chem Phys 115:2846–2859
Padding J, Briels WJ (2002) Time and length scales of polymer melts studied by coarse-grained molecular dynamics simulations. J Chem Phys 117:925–943
Padding J, Briels WJ (2011) Systematic coarse-graining of the dynamics of entangled polymer melts: the road from chemistry to rheology. J Phys Condens Matter 23:233101
Paul W, Yoon DY, Smith GD (1995) An optimized united atom model for simulations of polymethylene melts. J Chem Phys 103:1702–1709
Peter C, Kremer K (2009) Multiscale simulation of soft matter systems – from the atomistic to the coarse-grained level and back. Soft Matter 5:4357–4366
Peters BL, Salerno KM, Agrawal A, Perahia D, Grest GS (2017) Coarse grained modeling of polyethylene melts: effect on dynamics. J Chem Theory Comp 13:2890–2896
Peters BL, Salerno KM, Ge T, Perahia D, Grest GS (2018) Dynamics of polydispersed, entangled polymer melts. in preparation
Plimpton S (1995) Fast parallel algorithms for short-range molecular dynamics. J Comput Phys 117:1–19
Reith D, Pütz M, Müller-Plathe F (2003) Deriving effective mesoscale potentials from atomistic simulations. J Comput Chem 24:1624–1636
Richter D, Butera R, Fetters L, Huang J, Farago B, Ewen B (1992) Entanglement constraints in polymer melts. A neutron spin echo study. Macromolecules 25:6156–6164
Salerno KM, Bernstein N (2018) Persistence length, end-end distance and structure of coarse-grained polymers. J Chem Theory Comp 14:2219–2229
Salerno KM, Agrawal A, Perahia D, Grest GS (2016a) Resolving dynamic properties of polymers through coarse-grained computational studies. Phys Rev Lett 116:058302
Salerno KM, Agrawal A, Peters BL, Perahia D, Grest GS (2016b) Dynamics in entangled polyethylene melts. Euro Phys J Special Topics 225:1707–1722
Schleger P, Farago B, Lartigue C, Kollmar A, Richter D (1998) Clear evidence of reptation in polyethylene from neutron spin-echo spectroscopy. Phys Rev Lett 81:124–127
Siepmann JI, Karaborni S, Smit B (1993) Simulating the critical properties of complex fluids. Nature 365:330–332
Sirk TW, Slizoberg YR, Brennan JK, Lisal M, Andzelm JW (2012) An enhanced entangled polymer model for dissipative particle dynamics. J Chem Phys 136:134903
Siu SW, Pluhackova K, Böckmann RA (2012) Optimization of the OPLS-AA force field for long hydrocarbons. J Chem Theory Comp 8:1459–1470
Sun Q, Faller R (2005) Systematic coarse-graining of atomistic models for simulation of polymeric systems. Comput Chem Eng 29:2380–2385
Vega JF, Rastogi S, Peters GWM, Meijer HEH (2004) Rheology and reptation of linear polymers. Ultrahigh molecular weight chain dynamics in the melt. J Rheol 48:663–678
Voth GA (2008) Coarse-graining of condensed phase and biomolecular systems. CRC press, Boca Raton
Wang H, Junghans C, Kremer K (2009) Comparative atomistic and coarse-grained study of water: what do we lose by coarse-graining? Euro Phys J E 28:221–229
Acknowledgments
KMS was supported in part by the National Research Council Associateship Program at the US Naval Research Laboratory. DP kindly acknowledged NSF DMR1611136 for partial support. This work was supported by the Sandia Laboratory Directed Research and Development Program. Research was carried out in part at the Center for Integrated Nanotechnologies, a US Department of Energy Office of Basic Energy Sciences user facility. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology and Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the US Department of Energy’s National Nuclear Security Administration under Contract DE-NA-0003525.
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Grest, G.S., Michael Salerno, K., Peters, B.L., Ge, T., Perahia, D. (2020). Resolving Properties of Entangled Polymers Melts Through Atomistic Derived Coarse-Grained Models. In: Andreoni, W., Yip, S. (eds) Handbook of Materials Modeling. Springer, Cham. https://doi.org/10.1007/978-3-319-44677-6_34
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DOI: https://doi.org/10.1007/978-3-319-44677-6_34
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