Abstract
Cholesteric mesophases based on cellulose ethers, such as ethyl cellulose and hydroxypropyl cellulose, have been studied widely for their remarkable ability to display macroscopic structural color. However, the typical time scales involved in the multiscale self-assembly of cholesteric liquid crystals, from individual nanoscale helical arrangements to discrete microscopic domains, and their dependence on the gel’s viscoelastic properties remain underexplored. Here, we establish a quantitative relationship between the kinetics of structural color formation after shear deformation and cholesteric order development at the nano- and microscales. Utilizing rheology in tandem with static and time-resolved reflectivity measurements, we underscore the strong influence of polymer diffusivity and chain elasticity on self-assembly kinetics in cholesteric cellulose ether gels. We show that our phenomenological model can be employed to assess the structure-property relationships of multiple polysaccharide systems, elucidating key design guidelines for the development and processing of structurally colored cholesteric mesophases.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 4977-4990 |
| Number of pages | 14 |
| Journal | Biomacromolecules |
| Volume | 25 |
| Issue number | 8 |
| DOIs | |
| State | Published - Aug 12 2024 |
Funding
The authors thank Matthew Thompson and Prof. Nathan Gianneschi for their assistance with gel-permeation chromatography measurements, Kush Patel and Prof. Jeffrey Richards for their valuable input on the rheological studies, and members of the Sustainable Polymer Innovation (SPIn) Lab for their support. S.G.F. gratefully acknowledges support from the Ryan Fellowship and the International Institute for Nanotechnology (IIN) at Northwestern University. S.E.B. gratefully acknowledges support from the NU-MRSEC (NSF award no. DMR-2308691). This work made use of the MatCI Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University. This work made use of the EPIC facility of Northwestern University\u2019s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN, and Northwestern\u2019s MRSEC program (NSF DMR-2308691). This work made use of the IMSERC NMR facility at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-2025633), the IIN, and Northwestern University. The authors also acknowledge partial support for supplies provided by Leslie and Mac McQuown through a seed grant from the Center for Engineering Sustainability and Resilience at NU.
ASJC Scopus subject areas
- Bioengineering
- Biomaterials
- Polymers and Plastics
- Materials Chemistry