Multiscale Rheo-Optical and Scattering Signatures of Deformation-Induced Anisotropy in Aqueous Cellulose Nanocrystal Suspensions under Large-Amplitude Oscillatory Shear.
4 affiliations
- 1Business Unit Characterization, Anton Paar Japan K. K., 1st fl., Riverside Sumida, Tsutsumi-dori 1-19-9, Sumida-ku, Tokyo131-0034, Japan.
- 2Research Institute for Science and Technology, Tokyo University of Science, 2641 Yamazaki, Noda-shi, Chiba278-8510, Japan.
- 3Anton Paar Malaysia Sdn Bhd, 6, Jalan Perpustakawan U1/62, Temasya Glenmarie, Seksyen U1, 40150, Shah Alam, SelangorMalaysia.
- 4Photonic Lattice, Inc., LABO CITY SENDAI, 6-6-3 Minami-Yoshinari, Aoba-Ku, Sendai-City, Miyagi989-3204, Japan.
Abstract
Aqueous surface-charged cellulose nanocrystal (CNC) suspensions exhibit concentration-dependent viscosity growth, gelation, and deformation-induced anisotropy, but the concentration and strain-amplitude ranges over which these responses emerge are not necessarily the same. Here, low-shear rheology and linear viscoelasticity are combined with rheo-polarized imaging (Rheo-PI) and rheo-small-angle light scattering (Rheo-SALS) to compare mechanical, optical, and scattering signatures in the same CNC system. Analysis of the operational low-rate viscosity and the Winter-Chambon criterion separates an empirical viscosity-crossover concentration, Ccross, from the sol-gel transition concentration, Cg. Under fixed-frequency large-amplitude oscillatory shear (LAOS), nonphase-resolved but directly comparable Rheo-PI and Rheo-SALS readouts show that annularly averaged Rheo-PI retardation becomes detectable at lower concentrations and lower strain amplitudes than those required for the appearance of anisotropic X-shaped SALS patterns. The first optical transition approximately coincides with an apparent contraction of initially circular SALS patterns, whereas clearly directional X-shaped SALS patterns appear only at larger strain amplitudes. The X-shaped lobe geometry then evolves continuously with the strain amplitude, providing a later SALS-based signature of directional mesoscopic anisotropy under the imposed LAOS conditions. Together, these results provide a comparative multiscale map of deformation-induced anisotropy in CNC suspensions and distinguish viscosity crossover, gelation, local optical anisotropy, mechanical yielding, and anisotropic scattering signatures as related but noncoincident responses.
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BibTeX
@article{yamagata2026multiscale,
title = {{Multiscale Rheo-Optical and Scattering Signatures of Deformation-Induced Anisotropy in Aqueous Cellulose Nanocrystal Suspensions under Large-Amplitude Oscillatory Shear.}},
author = {Yoshifumi Yamagata and Ainaa Amirah Marzuki and Saki Otobe and Moe Araida and Taisuke Sato},
journal = {Langmuir : the ACS journal of surfaces and colloids},
year = {2026},
month = oct,
doi = {10.1021/acs.langmuir.6c03702},
url = {https://europepmc.org/article/MED/42918143},
note = {CC BY},
}
RIS
TY - JOUR
TI - Multiscale Rheo-Optical and Scattering Signatures of Deformation-Induced Anisotropy in Aqueous Cellulose Nanocrystal Suspensions under Large-Amplitude Oscillatory Shear.
AU - Yoshifumi Yamagata
AU - Ainaa Amirah Marzuki
AU - Saki Otobe
AU - Moe Araida
AU - Taisuke Sato
PY - 2026
DA - 2026/10/01
JO - Langmuir : the ACS journal of surfaces and colloids
DO - 10.1021/acs.langmuir.6c03702
UR - https://europepmc.org/article/MED/42918143
AB - Aqueous surface-charged cellulose nanocrystal (CNC) suspensions exhibit concentration-dependent viscosity growth, gelation, and deformation-induced anisotropy, but the concentration and strain-amplitude ranges over which these responses emerge are not necessarily the same. Here, low-shear rheology and linear viscoelasticity are combined with rheo-polarized imaging (Rheo-PI) and rheo-small-angle light scattering (Rheo-SALS) to compare mechanical, optical, and scattering signatures in the same CNC system. Analysis of the operational low-rate viscosity and the Winter-Chambon criterion separates an empirical viscosity-crossover concentration, Ccross, from the sol-gel transition concentration, Cg. Under fixed-frequency large-amplitude oscillatory shear (LAOS), nonphase-resolved but directly comparable Rheo-PI and Rheo-SALS readouts show that annularly averaged Rheo-PI retardation becomes detectable at lower concentrations and lower strain amplitudes than those required for the appearance of anisotropic X-shaped SALS patterns. The first optical transition approximately coincides with an apparent contraction of initially circular SALS patterns, whereas clearly directional X-shaped SALS patterns appear only at larger strain amplitudes. The X-shaped lobe geometry then evolves continuously with the strain amplitude, providing a later SALS-based signature of directional mesoscopic anisotropy under the imposed LAOS conditions. Together, these results provide a comparative multiscale map of deformation-induced anisotropy in CNC suspensions and distinguish viscosity crossover, gelation, local optical anisotropy, mechanical yielding, and anisotropic scattering signatures as related but noncoincident responses.
SN - 0743-7463
SN - 1520-5827
ER -