Date of Award

Spring 2015

Degree Type


Degree Name

Doctor of Philosophy (PhD)


Materials Engineering

First Advisor

Jeffrey Youngblood

Committee Chair

Jeffrey Youngblood

Committee Co-Chair

Robert Moon

Committee Member 1

Carlos Martinez

Committee Member 2

John Howarter


The biorenewable nature of cellulose nanocrystals (CNCs) has opened up new opportunities for cost-effective, sustainable materials design. By taking advantage of their distinctive structural properties and self-assembly, promising applications have started to nurture the fields of flexible electronics, biomaterials, and nanocomposites. CNCs exhibit two fundamental characteristics: rod-like morphology (5-20 nm wide, 50-500 nm long), and lyotropic behavior (i.e., liquid crystalline mesophases formed in solvents), which offer unique opportunities for structural control and fine tuning of thermal and optical properties based on a proper understanding of their individual behavior and interactions at different length scales. In the present work, we attempt to provide an integral description of the influence of single crystals in the thermal and optical response exhibited by nanostructured films. Our approach involved the connection of experimental evidence with predictions of molecular dynamics (MD) simulations. In order to assess the effect of CNC orientation in the bulk response, we produced cellulose nanostructured films under two different mechanisms, namely, self-organization and shear orientation. Self-organized nanostructured films exhibited the typical iridescent optical reflection generated by chiral nematic organization. Shear oriented films disrupted the cholesteric organization, generating highly aligned structures with high optical transparency. The resultant CNC organization present in all nanostructured films was estimated by a second order statistical orientational distribution based on two- dimensional XRD signals. A new method to determine the coefficient of thermal expansion (CTE) in a contact-free fashion was developed to properly characterize the thermal expansion of thin soft films by excluding other thermally activated phenomena. The method can be readily extended to other soft materials to accurately measure thermal strains in a non-destructive way. By evaluating the magnitude of film CTEs relative to those of individual CNC crystals, we highlighted the significant role played by crystalline interfaces. Likewise, after measuring the thermal conductivity of a single crystal and CNC films having multiple organizations, the interfacial thermal resistance arose as a governing factor for heat transport. We will offer further insights into the intricate connection of thermal and optical properties towards a future efficient manufacture and optimal CNC based-materials design