Douglas J. Grzetic CAP Congress 2014 Advisor: Robert A. Wickham
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Transcript of Douglas J. Grzetic CAP Congress 2014 Advisor: Robert A. Wickham
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Dynamical self-consistent field theory for kinetics of structure formation in dense polymeric
systemsDouglas J. Grzetic
CAP Congress 2014
Advisor: Robert A. Wickham
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Introduction
particle-based simulation(MD, Brownian dynamics)
coarse-grained field theories(DFT, tdGL, etc)
• Interacting many-body problem
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Introduction
particle-based simulation(MD, Brownian dynamics)
coarse-grained field theories(DFT, tdGL, etc)?
• Interacting many-body problem
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First-principles microscopic dynamics
drag force spring force “Fspr” non-bondedinteraction force
random force
• Many-body interacting Langevin equation
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Dynamical self-consistent field theory
• Dynamical mean-field approximation
• Derived from first-principles microscopic dynamicsD. J. Grzetic, R. A. Wickham and A.-C. Shi, Statistical dynamics of classical systems: A self-consistent field approach, J. Chem. Phys. (2014, in press)
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Potential applications to dynamical problems
colloidal dynamics
active matter
entangled chain dynamics
phase separation kineticshttp://www.nonmet.mat.ethz.ch/research/Colloidal_Chemistry_Ceramic_Processing/Colloid_Chemistry.jpg
R. K. W. Spencer and R. A. Wickham, Soft Matter (2013)http://upload.wikimedia.org/wikipedia/commons/3/32/EscherichiaColi_NIAID.jpg
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Potential applications to dynamical problems
colloidal dynamics
active matter
entangled chain dynamics
phase separation kineticshttp://www.nonmet.mat.ethz.ch/research/Colloidal_Chemistry_Ceramic_Processing/Colloid_Chemistry.jpg
R. K. W. Spencer and R. A. Wickham, Soft Matter (2013)http://upload.wikimedia.org/wikipedia/commons/3/32/EscherichiaColi_NIAID.jpg
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D. J. Grzetic, R. A. Wickham and A.-C. Shi, Statistical dynamics of classical systems: A self-consistent field approach, J. Chem. Phys. (2014, in press)
Dynamical self-consistent field theory
density:
mean field:
functional Smoluchowski equation:
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D. J. Grzetic, R. A. Wickham and A.-C. Shi, Statistical dynamics of classical systems: A self-consistent field approach, J. Chem. Phys. (2014, in press)
Dynamical self-consistent field theory
density:
mean field:
functional Smoluchowski equation:
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• Equivalent Langevin simulation of chain dynamics (1.6 million chain ensemble)
• Parallelizable (~1 day run time, 32 cores)
Single-chain dynamics in a mean field
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• Truncated Lennard-Jones interaction
Microscopic (non-bonded) bead-bead interaction
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Symmetric polymer blend: spinodal decomposition
spinodal
BA
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Onset of macro-phase separation:structure factor
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Microphase separation in AB diblock copolymers
timescale ~102tR
BAasymmetric
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Order-order transition: structure factor
rA - rB structure factor
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Chain configuration statistics: Rg map
rA - rB radius of gyration, A block
more stretched
less stretched
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Conclusions• Demonstrated ability to study kinetics of
macro/microphase separation in large, dense inhomogeneous polymer systems
• Truly non-equilibriummean field theory
• Connection to microscopicdynamics (Rg, tR)
• Retain chain conformationstatistics
D. J. Grzetic, R. A. Wickham and A.-C. Shi, Statistical dynamics of classical systems: A self-consistent field approach, J. Chem. Phys. (2014, in press)