A comprehensive study on intrinsic alpha corpuscular radiation damage in monazite crystals using picometer-scale imaging, coupled with SCXRD and Raman spectroscopy

Abstract

We have investigated monazite crystals, known to experience lattice distortions due to alpha particle emission from their atomic nuclei. Our aim in this investigation is to study the complex relationship between the lattice parameters and Raman spectra of monazite crystals. Through this study, we seek to understand the interdependency between these physical parameters and their influence on one another for an improved understanding of radiation-induced damage in these crystals. In addition to this, we also attempted to establish a correlation between these properties and their picometer-scale images to gain a deeper understanding of the structural changes that occur at the atomic scale. We conducted our study on four monazite samples withstanding intrinsic alpha decay radiation, denoted as M1, M2, M3, and M4, with crystal unit cell volume ranging from 299.961 Å3 to 301.96 Å3. Our Pearson statistical analysis revealed a correlation R2 (0.96) between the SCXRD-derived Ce–P Distance of monazite and the FWHM of PO4 band active mode in Raman spectra. This indicated lattice distortions due to alpha decay radiation impacting the Raman spectra. While Raman PO4 band broadening can be a consequence of impurities, dopants, and radiation damage, HRTEM scrutiny of the samples at picometer scales revealed the presence of point defects, plane rotation, and lattice distortions within the samples, suggesting the impact of alpha decay on the crystal lattice. HRTEM analysis has added additional confirmation that the major contribution to PO4 band broadening is due to alpha radiation damage in these samples. Through our study, we conclude a multiple-approach correlation is necessary to accurately study radiation damage dynamics at atomic scales.