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Title: Development of a PointNet for Detecting Morphologies of Self-Assembled Block Oligomers in Atomistic Simulations
ABSTRACT: Molecular simulations with atomistic or coarse- 6 grained force fields are a powerful approach for understanding and 7 predicting the self-assembly phase behavior of complex molecules. 8 Amphiphiles, block oligomers, and block polymers can form 9 mesophases with different ordered morphologies describing the 10 spatial distribution of the blocks, but entirely amorphous nature for 11 local packing and chain conformation. Screening block oligomer 12 chemistry and architecture through molecular simulations to find 13 promising candidates for functional materials is aided by effective 14 and straightforward morphology identification techniques. Captur- 15 ing 3-dimensional periodic structures, such as ordered network 16 morphologies, is hampered by the requirement that the number of 17 molecules in the simulated system and the shape of the periodic simulation box need to be commensurate with those of the resulting 18 network phase. Common strategies for structure identification include structure factors and order parameters, but these fail to 19 identify imperfect structures in simulations with incorrect system sizes. Building upon pioneering work by DeFever et al. [Chem. Sci. 20 2019, 10, 7503−7515] who implemented a PointNet (i.e., a neural network designed for computer vision applications using point 21 clouds) to detect local structure in simulations of single-bead particles and water molecules, we present a PointNet for detection of 22 nonlocal ordered morphologies of complex more » block oligomers. Our PointNet was trained using atomic coordinates from molecular 23 dynamics simulation trajectories and synthetic point clouds for ordered network morphologies that were absent from previous 24 simulations. In contrast to prior work on simple molecules, we observe that large point clouds with 1000 or more points are needed 25 for the more complex block oligomers. The trained PointNet model achieves an accuracy as high as 0.99 for globally ordered 26 morphologies formed by linear diblock, linear triblock, and 3-arm and 4-arm star-block oligomers, and it also allows for the discovery 27 of emerging ordered patterns from nonequilibrium systems. « less
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The journal of physical chemistry
Sponsoring Org:
National Science Foundation
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