Flexible and Responsive Chiral Nematic Cellulose Nanocrystal/Poly(ethylene glycol) Composite Films with Uniform and Tunable Structural Color

The fabrication of responsive photonic structures from cellulose nanocrystals (CNCs) that can operate in the entire visible spectrum is challenging due to the requirements of precise periodic modulation of the pitch size of the self‐assembled multilayer structures at the length scale within the wavelength of the visible light. The surface charge density of CNCs is an important factor in controlling the pitch size of the chiral nematic structure of the dried solid CNC films. The assembly of poly(ethylene glycol) (PEG) together with CNCs into smaller chiral nematic domains results in solid films with uniform helical structure upon slow drying. Large, flexible, and flat photonic composite films with uniform structure colors from blue to red are prepared by changing the composition of CNCs and PEG. The CNC/PEG(80/20) composite film demonstrates a reversible and smooth structural color change between green and transparent in response to an increase and decrease of relative humidity between 50% and 100% owing to the reversible swelling and dehydration of the chiral nematic structure. The composite also shows excellent mechanical and thermal properties, complementing the multifunctional property profile.