Molecular Dynamics Simulation and PRISM Theory Study
of Assembly in Solutions of Amphiphilic Bottlebrush Block Copolymers
Posted on 2018-09-20 - 18:35
We
use a coarse-grained model with both Polymer Reference Interaction
Site Model (PRISM) theory and molecular dynamics (MD) simulations
to study self-assembly of amphiphilic bottlebrush block copolymers
(BCPs) in solution as a function of increasing solvophobicity of the
solvophobic blocks. First, we evaluate the ability of PRISM theory
to describe and predict structure (e.g., intermolecular pair correlation
functions and structure factors) and thermodynamics (e.g., disorder
to order/assembled state transition solvophobicity and critical micelle
concentration) for solutions of bottlebrush BCPs for varying BCP sequence,
composition and solution concentration. Direct comparison of intermolecular
pair correlation functions and structure factors from PRISM theory
with that from MD simulations shows excellent qualitative, with some
quantitative, agreement. Additionally, PRISM theory results at low
solvophobicities present signatures of the structures observed in
MD simulations at higher solvophobicities. Comparisons of micro- and
macrophase peaks of structure factors obtained from PRISM theory at
low solvophobicities at various concentrations for linear and bottlebrush
BCPs predict that linear BCPs have a lower critical micelle concentration
(CMC) than bottlebrushes at the same molecular weight. These computationally
less intensive theoretical predictions are confirmed by results from
computationally more intensive MD simulations. Comparison of the microphase
peak positions in the structure factors obtained from PRISM theory
suggests that the bottlebrush BCPs form smaller micelles than linear
BCPs at the same molecular weight, which is also confirmed visually
and through cluster analysis of trajectories from MD simulations.
Through this study, we show the power of using theory and simulations
in an integrated and sequential manner to quickly explore a large
set of soft materials design parameters for desired assembly.
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Lyubimov, Ivan; Wessels, Michiel G.; Jayaraman, Arthi (2018). Molecular Dynamics Simulation and PRISM Theory Study
of Assembly in Solutions of Amphiphilic Bottlebrush Block Copolymers. ACS Publications. Collection. https://doi.org/10.1021/acs.macromol.8b01535
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AUTHORS (3)
IL
Ivan Lyubimov
MW
Michiel G. Wessels
AJ
Arthi Jayaraman
KEYWORDS
PRISM Theory StudyMolecular Dynamics Simulationstructure factorsPRISM theorysolutionCMCbottlebrush BCPs formPRISM theory resultsbottlebrush BCPsamphiphilic bottlebrush block copolymersmicelle concentrationsolvophobicitieAmphiphilic Bottlebrush Block CopolymersMD simulationsPolymer Reference Interaction Site Modelpair correlation functionsmicrophase peak positionsmaterials design parameters