Priming self-assembly pathways by stacking block copolymers

Russell, Sebastian T.; Bae, Suwon; Subramanian, Ashwanth; Tiwale, Nikhil; Doerk, Gregory; Nam, Chang-Yong; Fukuto, Masafumi; Yager, Kevin G.

doi:10.1038/s41467-022-34729-0

Priming self-assembly pathways by stacking block copolymers

Journal Article · Sun Nov 13 23:00:00 EST 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-022-34729-0· OSTI ID:1898231

; ; Subramanian, Ashwanth; ; ; ; Fukuto, Masafumi;

Abstract

Block copolymers spontaneously self-assemble into well-defined nanoscale morphologies. Yet equilibrium assembly gives rise to a limited set of structures. Non-equilibrium strategies can, in principle, expand diversity by exploiting self-assembly’s responsive nature. In this vein, we developed a pathway priming strategy combining control of thin film initial configurations and ordering history. We sequentially coat distinct materials to form prescribed initial states, and use thermal annealing to evolve these manifestly non-equilibrium states through the assembly landscape, traversing normally inaccessible transient structures. We explore the enormous associated hyperspace, spanning processing (annealing temperature and time), material (composition and molecular weight), and layering (thickness and order) dimensions. We demonstrate a library of exotic non-native morphologies, including vertically-oriented perforated lamellae, aqueduct structures (vertical lamellar walls with substrate-pinned perforations), parapets (crenellated lamellae), and networks of crisscrossing lamellae. This enhanced structural control can be used to modify functional properties, including accessing regimes that surpass their equilibrium analogs.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0012704

OSTI ID:: 1898231

Alternate ID(s):: OSTI ID: 1922718

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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