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In silico study on probing atomistic insights into structural stability and tensile properties of Fe-doped hydroxyapatite single crystals

Basu, S and Nag, S and Kottan, NB and Basu, B (2022) In silico study on probing atomistic insights into structural stability and tensile properties of Fe-doped hydroxyapatite single crystals. In: Scientific Reports, 12 (1).

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Official URL: https://doi.org/10.1038/s41598-022-24904-0


Hydroxyapatite (HA, Ca10PO4(OH)2) is a widely explored material in the experimental domain of biomaterials science, because of its resemblance with natural bone minerals. Specifically, in the bioceramic community, HA doped with multivalent cations (e.g., Mg2+, Fe2+, Sr2+, etc.) has been extensively investigated in the last few decades. Experimental research largely established the critical role of dopant content on mechanical and biocompatibility properties. The plethora of experimental measurements of mechanical response on doped HA is based on compression or indentation testing of polycrystalline materials. Such measurements, and more importantly the computational predictions of mechanical properties of single crystalline (doped) HA are scarce. On that premise, the present study aims to build atomistic models of Fe2+-doped HA with varying Fe content (10, 20, 30, and 40 mol%) and to explore their uniaxial tensile response, by means of molecular dynamics (MD) simulation. In the equilibrated unit cell structures, Ca(1) sites were found to be energetically favourable for Fe2+ substitution. The local distribution of Fe2+ ions significantly affects the atomic partial charge distribution and chemical symmetry surrounding the functional groups, and such signatures are found in the MD analyzed IR spectra. The significant decrease in the intensity of the IR bands found in the Fe-doped HA together with band splitting, because of the symmetry changes in the crystal structure. Another important objective of this work is to computationally predict the mechanical response of doped HA in their single crystal format. An interesting observation is that the elastic anisotropy of undoped HA was not compromised with Fe-doping. Tensile strength (TS) is systematically reduced in doped HA with Fe2+ dopant content and a decrease in TS with temperature can be attributed to the increased thermal agitation of atoms at elevated temperatures. The physics of the tensile response was rationalized in terms of the strain dependent changes in covalent/ionic bond framework (Ca–P distance, P–O bond strain, O–P–O angular strain, O–H bond distance). Further, the dynamic changes in covalent bond network were energetically analyzed by calculating the changes in O–H and P–O bond vibrational energy. Summarizing, the current work establishes our foundational understanding of the atomistic phenomena involved in the structural stability and tensile response of Fe-doped HA single crystals.

Item Type: Journal Article
Publication: Scientific Reports
Publisher: Nature Research
Additional Information: The copyright for this article belongs to the Author(S).
Department/Centre: Division of Chemical Sciences > Materials Research Centre
Division of Chemical Sciences > Solid State & Structural Chemistry Unit
Division of Interdisciplinary Sciences > Centre for Biosystems Science and Engineering
Date Deposited: 09 Jan 2023 06:44
Last Modified: 09 Jan 2023 06:44
URI: https://eprints.iisc.ac.in/id/eprint/78896

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