journal article·2025-02Open access

Propagation of Orientation Across Lengthscales in Sheared Self‐Assembling Hierarchical Suspensions via Rheo‐PLI‐SAXS

Reza Ghanbari, Ann Terry, Sylwia Wojno, Marko Bek, Kesavan Sekar, Amit Kumar Sonker, Kim Nygård, Viney Ghai, Simona Bianco, Marianne Liebi, Aleksandar Matic, Gunnar Westman, Tiina Nypelö, Roland Kádár

Advanced Science· Volume 12· Issue 7

Abstract

Abstract Simultaneous rheological, polarized light imaging, and small‐angle X‐ray scattering experiments (Rheo‐PLI‐SAXS) are developed, thereby providing unprecedented level of insight into the multiscale orientation of hierarchical systems in simple shear. Notably, it is observed that mesoscale alignment in the flow direction does not develop simultaneously across nano‐micro lengthscales in sheared suspensions of rod‐like chiral‐nematic (meso) phase forming cellulose nanocrystals. Rather, with increasing shear rate, orientation is observed first at mesoscale and then extends to the nanoscale, with influencing factors being the aggregation state of the hierarchy and concentration. In biphasic systems, where an isotropic phase co‐exists with self‐assembled liquid crystalline mesophase domains, the onset of mesodomain alignment towards the flow direction can occur at shear rates nearing one decade before a progressive increase in preferential orientation at nanoscale is detected. If physical confinement prevents the full formation of a cholesteric phase, mesoscale orientation occurs in shear rate ranges that correspond to de‐structuring at nanoscale. Interestingly, nano‐ and mesoscale orientations appear to converge only for biphasic suspensions with primary nanoparticles predominantly made up of individual crystallites and in a high‐aspect ratio nematic‐forming thin‐wall nanotube system. The nano‐micro orientation propagation is attributed to differences in the elongation and breakage of mesophase domains.
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Research context

OpenAlex topics: Advanced Cellulose Research Studies · Liquid Crystal Research Advancements · Advanced Materials and Mechanics

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Industrial and Materials Science, Division of Engineering Materials Chalmers University of Technology Gothenburg SE‐412 96 Sweden

MAX IV Laboratory Lund University Lund SE‐224 84 Sweden

LINXS Institute of advanced Neutron and X‐ray Science (LINXS) Scheelevägen 19 Lund 223 70 Sweden

Wallenberg Wood Science Centre (WWSC) Chalmers University of Technology Gothenburg SE‐412 96 Sweden

School of Chemistry University of Glasgow Glasgow G12 8QQ UK

Department of Physics, Division of Materials Physics Chalmers University of Technology Gothenburg SE‐412 96 Sweden

Paul Scherrer Institute Division of Photon Science Villigen CH‐5232 Switzerland

Institute of Materials Ecole Polytechnique Fédérale de Lausanne (EPFL) Lausanne CH‐1015 Switzerland

Department of Chemistry and Chemical Engineering, Division of Organic Chemistry Chalmers University of Technology Gothenburg SE‐412 96 Sweden

Department of Chemistry and Chemical Engineering, Division of Applied Chemistry Chalmers University of Technology Gothenburg SE‐412 96 Sweden

Department of Bioproducts and Biosystems Aalto University Espoo FI‐00760 Finland

Funding

Stiftelsen Chalmers tekniska högskola · Wallenberg Wood Science Center · Vinnova · Nanoscience and Nanotechnology Area of Advance, Chalmers Tekniska Högskola

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