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From Molecules to Materials: Engineering New Ionic Liquid Crystals Through Halogen Bonding

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Ionic liquid as a structure-directing agent for Frank-Kasper phase formation in block copolymers.

Aditya Sahare¹, Sumana Bandyopadhyay¹, Yu-Hsuan Lin²

¹Department of Chemical Engineering, National Tsing Hua University, Hsinchu, Taiwan, ROC.

Nature Communications

|June 2, 2026

Summary

Ionic liquids enable complex Frank-Kasper phases in block copolymers. This study shows incorporating 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIM][TFSI]) into PEO-b-PB creates tunable, reconfigurable spherical micelle structures.

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Area of Science:

Materials Science
Polymer Chemistry
Soft Matter Physics

Background:

Accessing complex Frank-Kasper (FK) phases in block copolymers (BCPs) typically involves intricate molecular engineering or polymer blending.
Existing methods present limitations in achieving diverse FK phase structures and tunability.

Purpose of the Study:

To demonstrate a facile and tunable method for accessing complex FK phases in BCPs.
To expand the phase space of spherical micelle packings using ionic liquids.
To investigate the role of ionic liquids in stabilizing FK lattices.

Main Methods:

Incorporation of the ionic liquid (IL), 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIM][TFSI]), into a cylinder-forming poly(ethylene oxide)-block-poly(1,2-butadiene) (PEO-b-PB) system.
Exploration of phase behavior across various compositions and temperatures.
Analysis of the IL's dual role in modifying polymer interactions and morphology.

Main Results:

Observation of diverse FK phases, including σ, A15, and Laves C15, over broad composition and temperature ranges.
Identification of thermotropic (A15 → σ → C15) and lyotropic (σ → A15 → C15) phase transition sequences.
Demonstration of the IL enhancing the effective Flory-Huggins parameter (χ) and inducing dry-brush segregation.

Conclusions:

The ionic liquid [EMIM][TFSI] acts as a versatile additive for stabilizing complex FK phases in a simple diblock copolymer system.
This approach provides a tunable and facile route to reconfigurable complex spherical micelle assemblies.
The findings offer new possibilities for designing advanced materials with ordered nanostructures.