Gregory, Grason
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Professor, Department Polymer Science and Engineering
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Gregory
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Grason
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Polymer and Organic Materials
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Publication Open Access Medial packing and elastic asymmetry stabilize the double-gyroid in block copolymers(2022-01-01) Reddy, Abhiram; Dimitriyev, Michael S; Grason, Gregory MTriply-periodic networks are among the most complex and functionally valuable self-assembled morphologies, yet they form in nearly every class of biological and synthetic soft matter building blocks. In contrast to simpler assembly motifs – spheres, cylinders, layers – networks require molecules to occupy variable local environments, confounding attempts to understand their formation. Here, we examine the double-gyroid network phase by using a geometric formulation of the strong stretching theory of block copolymer melts, a prototypical soft self-assembly system. The theory establishes the direct link between molecular packing, assembly thermodynamics and the medial map, a generic measure of the geometric center of complex shapes. We show that “medial packing” is essential for stability of double-gyroid in strongly-segregated melts, reconciling a long-standing contradiction between infinite- and finite-segregation theories. Additionally, we find a previously unrecognized non-monotonic dependence of network stability on the relative entropic elastic stiffness of matrix-forming to tubular-network forming blocks. The composition window of stable double-gyroid widens for both large and small elastic asymmetry, contradicting intuitive notions that packing frustration is localized to the tubular domains. This study demonstrates the utility of optimized medial tessellations for understanding soft-molecular assembly and packing frustration via an approach that is readily generalizable far beyond gyroids in neat block copolymers.Publication Open Access Data for Elastically-mediated Positioning of 2D Colloids(2021-01-01) Xin, Weiyue; Wu, Hao; Grason, Gregory M.; Santore, Maria M.; Gregory, Grason; Santore, Maria; Gregory, Grason; Santore, MariaData for publication “Elastically-mediated Positioning of 2D Colloids” by Weiyue Xin, Hao Wu, Gregory Grason, Maria Santore, 2021.Publication Open Access Source Data for Self-Spinning Filaments for Autonomously Linked Microfibers(2022-01-01) Barber, Dylan M; Emrick, Todd; Gregory, Grason; Crosby, AlFilamentous bundles are ubiquitous in Nature, achieving highly adaptive functions and structural integrity from assembly of diverse mesoscale supramolecular elements. Engineering routes to synthetic, topologically integrated analogs demands precisely coordinated control of multiple filaments’ shapes and positions, a major challenge when performed without complex machinery or labor-intensive processing. Here, we demonstrate a photocreasing design that encodes local curvature and twist into mesoscale polymer filaments, enabling their programmed transformation into target 3-dimensional geometries. Importantly, patterned photocreasing of filament arrays drives autonomous spinning to form linked filament bundles that are highly entangled and structurally robust. In individual filaments, photocreases unlock paths 16 to arbitrary, 3-dimensional curves in space. Collectively, photocrease-mediated bundling establishes a transformative paradigm enabling smart, self-assembled mesostructures that mimic performance-differentiating structures in Nature (e.g., tendon and muscle fiber) and the macro-engineered world (e.g., rope).Publication Open Access Source Data for Mingqiu Hu, Hong-Gyu Seong, Michael S. Dimitriyev, Weiguo Hu, Zhan Chen, Gregory M. Grason, Todd Emrick, and Thomas P. Russell, "Backbone chain stitching in bottlebrush statistical copolymers"(2024-01-01) Hu, Mingqiu; Seong, Hong-Gyu; Dimitriyev, Michael S.; Hu, Weiguo; Chen, Zhan; Gregory, Grason M.; Emrick, Todd S.; Russell, Thomas P.; Gregory, Grason; Emrick, Todd; Gregory, Grason; Emrick, ToddPublication Open Access Source data for "Flowering of Developable 2D Crystal Shapes in Closed, Fluid Membranes"(2024-01-01) Wan, Hao; Jeon, Geunwoong; Xin, Weiyue; Grason, Gregory M; Santore, Maria M; Gregory, Grason; Santore, Maria; Gregory, Grason; Santore, MariaSource data for "Flowering of Developable 2D Crystal Shapes in Closed, Fluid Membranes".Publication Open Access Source Data for "End exclusion zones in strongly stretched, molten polymer brushes of arbitrary shape"(2021-01-01) Dimitriyev, Michael S; Grason, Gregory M; Gregory, Grason; Gregory, GrasonSupplementary code for solving the constraint equations that describe curved polymer brushes. Also contains software for analyzing the resulting solutions.Publication Open Access Source Data for "Medial packing and elastic asymmetry stabilize the double-gyroid in block copolymers"(2022-01-01) Reddy, Anugu Abhiram; Dimittiyev, Michael S.; Gregory, Grason; Gregory, Grason; Gregory, GrasonSource code and data for "Medial packing and elastic asymmetry stabilize the double-gyroid in block copolymers." Readme included in zip file.Publication Open Access Supplementary Code for "Chain trajectories, domain shapes and terminal boundaries in block copolymers"(2023-01-01) Greenvall, Benjamin R; Dimitriyev, Michael S.; Grason, Gregory M; Gregory, Grason; Gregory, GrasonSupplementary code used for the publication "Chain trajectories, domain shapes and terminal boundaries in block copolymers" by Benjamin R. Greenvall, Michael S. Dimitriyev, and Gregory M. Grason. Includes code for extracting and analyzing polar order and chain trajectories from self-consistent field calculations of block copolymers.Publication Open Access Source Data for "Seeing mesoatomic distortions in soft-matter crystals of a double-gyroid block copolymer"(2019-01-01) Feng, Xueyan; Burke, Christopher; Zhou, Mujin; Gao, Hua; Yang, Kaiqi; Reddy, Abhiram; Prasad, Ishan; Ho, Rong-Ming; Avgeropoulos, Apostolos; Grason, Greg; Thomas, Edwin; Gregory, Grason; Gregory, GrasonPublication Open Access Source Data for "Block copolymers beneath the surface: measuring and molding complex morphology at the sub-domain scale"(2021-01-01) Reddy, Abhiram; Thomas, Edwin; Grason, Greg; Gregory, Grason; Gregory, Grason