Gradient Magnesium Content Affects Nanomechanics via Decreasing the Size and Crystallinity of Nanoparticles of Pseudoosteodentine of the Pacific Cutlassfish, Trichiurus lepturus Teeth

The formation of biomaterials such as enamel, dentin, and bone is important for many organisms, and the mechanical properties of biomaterials are affected by a wide range of structural and chemical factors. Special dentins exist in extant aquatic gnathostomes, and many more are present in fossils. When a layer of compact orthodentine surrounds the porous osteodentine core in the crown, the composite dentin is called pseudoosteodentine. Using various high-resolution analytical techniques, including micro-computed tomography (micro-CT), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), Raman spectroscopy, and nanoindentation, we analyzed the micro- and nanostructures, chemical composition, and mechanical properties of pseudoosteodentine in the Pacific cutlassfish, Trichiurus lepturus teeth. Nanoscale oval-shaped hydroxyapatite (HA) crystals were distributed in a disordered manner in the pseudoosteodentine, and a cross-sectional analysis showed that the mineral crystallinity and crystalline particle size of the outer orthodentine were greater than those of middle and inner osteodentine. Moreover, the outer orthodentine comprised a mixture of smaller crystals and larger, more mature crystals. The nano-hardness and nano-stiffness of outer orthodentine were significantly higher than those of middle and inner osteodentine along a radical direction. The hardness and stiffness of pseudoosteodentine were inversely proportional to its magnesium (Mg) content. These data are consistent with the concept that Mg delays crystal maturation. The crystal size, crystallinity, nano-hardness, and nano-stiffness of pseudoosteodentine all decreased commensurately with the increase of its Mg concentration. The pseudoosteodentine of T. lepturus also can be regarded as a functional gradient material (FGM) because its mechanical properties are closely related to its chemical composition and nanostructure. Special pseudoosteodentine may therefore serve as a design standard for biomimetic synthetic mineral composites.