Unexpected microphase transitions in flow towards nematic order of cellulose nanocrystals

Organization of nanoparticles is essential in order to control their light-matter interactions. We present cellulose nanocrystal suspension organization in flow towards a unidirectional state. Visualization of evolving polarization patterns of the cellulose nanocrystal suspensions is combined with steady and oscillatory shear rheology. Elucidation of the chiral nematic mesophase in a continuous process towards unidirectional order enables control of alignment in a suspension precursor for structural films and reveals thus far in situ unrevealed transition states that were not detectable by rheology alone. The coupled analytics enabled the suspensions of interest to be divided into rheological gels and rheological liquid crystal fluids with detailed information on the microtransition phases. Both populations experienced submicron organization and reached macro-scale homogeneity with unidirectional ordering in continued shear. We quantify the time, shear rate, and recovery time after shear to design an optimizing formation process for controlled wet structures as precursors for dry products. Graphic abstract