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Bone is mineralized tissue constituting the skeletal system, supporting andprotecting body organs and tissues. At the molecular level, mineralizedcollagen fibril is the basic building block of bone tissue, and hence,understanding bone properties down to fundamental tissue structures enables tobetter identify the mechanisms of structural failures and damages. Whileefforts have focused on the study of the micro- and macro-scale viscoelasticityrelated to bone damage and healing based on creep, mineralized collagen has notbeen explored on a molecular level. We report a study that aims atsystematically exploring the viscoelasticity of collagenous fibrils withdifferent mineralization levels. We investigate the dynamic mechanical responseupon cyclic and impulsive loads to observe the viscoelastic phenomena fromeither shear or extensional strains via molecular dynamics. We perform asensitivity analysis with several key benchmarks: intrafibrillar mineralizationpercentage, hydration state, and external load amplitude. Our results show agrowth of the dynamic moduli with an increase of mineral percentage, pronouncedat low strains. When intrafibrillar water is present, the material softens theelastic component but considerably increases its viscosity, especially at highfrequencies. This behaviour is confirmed from the material response uponimpulsive loads, in which water drastically reduces the relaxation timesthroughout the input velocity range by one order of magnitude, with respect tothe dehydrated counterparts. We find that upon transient loads, water has amajor impact on the mechanics of mineralized fibrillar collagen, being able toimprove the capability of the tissue to passively and effectively dissipateenergy, especially after fast and high-amplitude external loads.

Molecular origin of viscoelasticity in mineralized collagen fibrils