Crystalline cellulose elastic modulus predicted by atomistic models of uniform deformation and nanoscale indentation

The elastic modulus of cellulose Iβ in the axial and transverse directions was obtained from atomistic simulations using both the standard uniform deformation approach and a complementary approach based on nanoscale indentation. This allowed comparisons between the methods and closer connectivity to experimental measurement techniques. A reactive force field was used that explicitly describes hydrogen bond, coulombic and van der Waals interactions, allowing each contribution to the inter- and intra-molecular forces to be analyzed as a function of crystallographic direction. The uniform deformation studies showed that the forces dominating elastic behavior differed in the axial and transverse directions because of the relationship between the direction of the applied strain and the hydrogen bonding planes. Simulations of nanoscale indentation were then introduced to model the interaction between a hemispherical indenter with the \((1\bar{1}0)\) surface of a cellulose Iβ rod. The role of indenter size, loading force and indentation speed on the transverse elastic modulus was studied and, for optimized parameters, the results found to be in good agreement with experimentally-measured transverse elastic modulus for individual cellulose crystals.