Abstract
The interfaces that biological tissues form with biomaterials are invariably defective and frequently the location where failure initiates. Characterizing the phenomena that lead to failure is confounded by several factors including heterogeneous material/tissue interfaces. To seamlessly analyze across these diverse structures presents a wealth of analytical challenges. This study aims to develop a molecular-level understanding of a peptide-functionalized adhesive/collagen hybrid biomaterial using Raman spectroscopy combined with chemometrics approach. An engineered hydroxyapatite-binding peptide (HABP) was copolymerized in dentin adhesive and dentin was demineralized to provide collagen matrices that were partially infiltrated with the peptide-functionalized adhesive. Partial infiltration led to pockets of exposed collagen–a condition that simulates defects in adhesive/dentin interfaces. The spectroscopic results indicate that co-polymerizable HABP tethered to the adhesive promoted remineralization of the defects. The spatial distribution of collagen, adhesive, and mineral as well as crystallinity of the mineral across this heterogeneous material/tissue interface was determined using micro-Raman spectroscopy combined with chemometrics approach. The success of this combined approach in the characterization of material/tissue interfaces stems from its ability to extract quality parameters that are related to the essential and relevant portions of the spectral data, after filtering out noise and non-relevant information. This ability is critical when it is not possible to separate components for analysis such as investigations focused on, in situ chemical characterization of interfaces. Extracting essential information from complex bio/material interfaces using data driven approaches will improve our understanding of heterogeneous material/tissue interfaces. This understanding will allow us to identify key parameters within the interfacial micro-environment that should be harnessed to develop durable biomaterials.
Highlights
Clinical NeedUntreated dental caries of permanent teeth impact 2.3 billion people across the globe and more than 530 million children suffer from untreated dental caries of primary teeth (WHO, 2020)
These mineral-derived bands diminished in the demineralized dentin spectra, where spectral features assigned to dentin collagen became obvious, such as 1,003 cm−1 (C-C in phenyl group), 1,667 cm−1
We introduce a combined Raman spectroscopy and chemometrics approach to investigate heterogeneous material/tissue interfaces where biological cues were provided to promote tissue mineralization of deficient dentin matrices
Summary
Clinical NeedUntreated dental caries of permanent teeth impact 2.3 billion people across the globe and more than 530 million children suffer from untreated dental caries of primary teeth (WHO, 2020). The most popular material for the repair of lost or damaged tooth structure is dental composite (Ferracane, 2017; Eltahlah et al, 2018), but composite fails at a rate 2–3.5 times the rate of dental amalgam (Ferracane, 2013; Schwendicke et al, 2016; Afrashtehfar et al, 2017; Makvandi et al, 2018). Patients at high risk for caries, such as the 4 million United States children (Palmer, 2013) and more than 100 million adults (National Center for Health Statistics (US), 2007) who do not receive regular dental care, are vulnerable to composite-restoration failure and the downward spiral associated with frequent replacements (Kopperud et al, 2015; Schwendicke et al, 2016)
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