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The transfer of chirality across length-scales is an intriguing and universalnatural phenomenon. However, connecting the properties of individual buildingblocks to the emergent features of their resulting large-scale structureremains a challenge. In this work, we investigate the origins of mesophasechirality in cellulose nanocrystal suspensions, whose self-assembly into chiralphotonic films has attracted significant interest. By correlating the ensemblebehaviour in suspensions and films with a quantitative morphological analysisof the individual nanoparticles, we reveal an inverse relationship between thecholesteric pitch and the abundance of laterally-bound composite particles.These bundles thus act as colloidal chiral dopants, analogous to those used inmolecular liquid crystals, providing the missing link in the hierarchicaltransfer of chirality from the molecular to the colloidal scale.

Chiral Self-Assembly of Cellulose Nanocrystals is Driven by Crystallite Bundles