Hostname: page-component-cd9895bd7-gvvz8 Total loading time: 0 Render date: 2024-12-23T19:08:37.905Z Has data issue: false hasContentIssue false

A method for mapping submicron-scale crystallographic order/disorder applied to human tooth enamel

Published online by Cambridge University Press:  08 May 2020

R. Free*
Affiliation:
Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois, USA
K. DeRocher
Affiliation:
Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois, USA
R. Xu
Affiliation:
Argonne National Lab, Advanced Photon Source, Lemont, Illinois34ID-E, USA
D. Joester
Affiliation:
Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois, USA
S. R. Stock
Affiliation:
Northwestern University, Feinberg School of Medicine, Chicago, Illinois, USA
*
a)Author to whom correspondence should be addressed. Electronic mail: [email protected]

Abstract

Tooth enamel, the outermost layer of human teeth, is a complex, hierarchically structured biocomposite. The details of this structure are important in multiple human health contexts, from understanding the progression of dental caries (tooth decay) to understanding the process of amelogenesis and related developmental defects. Enamel is composed primarily of long, nanoscale crystallites of hydroxyapatite that are bundled by the thousands to form micron-scale rods. Studies with transmission electron microscopy show the relationships between small groups of crystallites and X-ray diffraction characterize averages over many rods, but the direct measurement of variations in local crystallographic structure across and between enamel rods has been missing. Here, we describe a synchrotron X-ray-based experimental approach and a novel analysis method developed to address this gap in knowledge. A ~500-nm-wide beam of monochromatic X-rays in conjunction with a sample section only 1 μm in thickness enables 2D diffraction patterns to be collected from small well-separated volumes within the enamel microstructure but still probes enough crystallites (~300 per pattern) to extract population-level statistics on crystallographic features like lattice parameter, crystallite size, and orientation distributions. Furthermore, the development of a quantitative metric to characterize relative order and disorder based on the azimuthal autocorrelation of diffracted intensity enables these crystallographic measurements to be correlated with their location within the enamel microstructure (e.g., between rod and interrod regions). These methods represent a step forward in the characterization of human enamel and will elucidate the variation of the crystallographic structure across and between enamel rods for the first time.

Type
Proceedings Paper
Copyright
Copyright © 2020 International Centre for Diffraction Data

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

Al-Jawad, M., Steuwer, A., Kilcoyne, S. H., Shore, R. C., Cywinski, R., and Wood, D. J. (2007). “2D mapping of texture and lattice parameters of dental enamel,” Biomaterials 28(18), 29082914.CrossRefGoogle ScholarPubMed
Al-Jawad, M., Addison, O., Khan, M. A., James, A., and Hendriksz, C. J. (2012). “Disruption of enamel crystal formation quantified by synchrotron microdiffraction,” J. Dent. 40(12), 10741080.CrossRefGoogle ScholarPubMed
Al-Mosawi, M., Davis, G. R., Bushby, A., Montgomery, J., Beaumont, J., and Al-Jawad, M. (2018). “Crystallographic texture and mineral concentration quantification of developing and mature human incisal enamel,” Sci. Rep. 8, 14449.CrossRefGoogle ScholarPubMed
Boyde, A. (1967). “The development of enamel structure,” Proc. R. Soc. Med. 60(9), 923928.Google ScholarPubMed
Boyde, A. (1976). “Amelogenesis and the structure of enamel,” in Scientific Foundations of Dentistry, edited by Cohen, B. and Kramer, I. R. (William Heinemann Medical Books Ltd, London), pp. 341343.Google Scholar
Glas, J. E. (1962). “Studies on the ultrastructure of dental enamel—II: The orientation of the apatite crystallites as deduced from x-ray diffraction,” Arch. Oral Biol. 7(1), 91104. IN15.CrossRefGoogle ScholarPubMed
Gordon, L. M., Cohen, M. J., MacRenaris, K. W., Pasteris, J. D., Seda, T., and Joester, D. (2015). “Amorphous intergranular phases control the properties of rodent tooth enamel,” Science 347(6223), 746750.CrossRefGoogle ScholarPubMed
Habelitz, S. (2015). “Materials engineering by ameloblasts,” J. Dent. Res. 94(6), 759767.CrossRefGoogle ScholarPubMed
Hammersley, A. P., Svensson, S. O., and Thompson, A. (1994). “Calibration and correction of spatial distortions in 2d detector systems,” Nucl. Instrum. Meth. Phys. Res. A 346, 312321.CrossRefGoogle Scholar
Hammersley, A. P., Svensson, S. O., Hanfland, M., Fitch, A. N., and Hausermann, D. (1996). “Two-dimensional detector software: from real detector to idealised image or two-theta scan,” High Pressure Res. 14, 235248.CrossRefGoogle Scholar
He, L. H. and Swain, M. V. (2007). “Enamel—a “metallic-like” deformable biocomposite,” J. Dent. 35(5), 431437.CrossRefGoogle Scholar
Kerebel, B., Daculsi, G., and Kerebel, L. M. (1979). “Ultrastructural studies of enamel crystallites,” J. Dent. Res. 58(2 suppl), 844851.CrossRefGoogle ScholarPubMed
Meckel, A. H., Griebstein, W. J., and Neal, R. J. (1965). “Structure of mature human dental enamel as observed by electron microscopy,” Arch. Oral Biol. 10, 775783.CrossRefGoogle ScholarPubMed
Nanci, A. (2012). Ten Cate's Oral Histology: Development, Structure, and Function (C.V. Mosby Co., St. Louis, MO).Google Scholar
Poole, D. F. G. and Brooks, A. W. (1961). “The arrangement of crystallites in enamel prisms,” Arch. Oral Biol. 5, 1426.CrossRefGoogle ScholarPubMed
Schneider, C. A., Rasband, W. S., and Eliceiri, K. W. (2012). “Nih image to imagej: 25 years of image analysis,” Nat. Methods 9, 671675.CrossRefGoogle ScholarPubMed
Simmons, L. M., Al-Jawad, M., Kilcoyne, S. H., and Wood, D. J. (2011). “Distribution of enamel crystallite orientation through an entire tooth crown studied using synchrotron X-ray diffraction,” Eur. J. Oral Sci. 119(s1), 1924.CrossRefGoogle ScholarPubMed
Xue, J., Zavgorodniy, A. V., Kennedy, B. J., Swain, M. V., and Li, W. (2013). “X-ray microdiffraction, TEM characterization and texture analysis of human dentin and enamel,” J. Microsc. 251(2), 144153.CrossRefGoogle ScholarPubMed
Yanagisawa, T., and Miake, Y. (2003). “High-resolution electron microscopy of enamel-crystal demineralization and remineralization in carious lesions,” Microscopy 52(6), 605613.CrossRefGoogle ScholarPubMed