Imaging neutron radiation-induced defects in single-crystal chemical vapor deposition diamond at the atomic level

Abstract

Diamond's exceptional properties make it highly suited for applications in challenging radiation environments. Understanding radiation-induced damage in diamond is crucial for enabling its practical applications and advancing materials science. However, direct imaging of radiation-induced crystal defects at the atomic scale remains rare due to diamond's compact lattice structure. Here, we report the atomic-level characterization of crystal defects induced by high-flux fast neutron radiation (up to $3 \times10^{17}$ n/$cm^2$) in single-crystal chemical vapor deposition diamonds. Through Raman spectroscopy, the phase transition from carbon $sp^3$ to $sp^2$ hybridization was identified, primarily associated with the formation of dumbbell-shaped interstitial defects. Using electron energy loss spectroscopy and aberration-corrected transmission electron microscopy, we observed a clustering trend in defect distribution, where $sp^2$ rich clusters manifested as dislocation structures with a density up to $10^{14}$ $cm^{-2}$. Lomer-Cottrell junctions were identified, offering a possible explanation for defect cluster formation. Radiation-induced point defects were found to be dispersed throughout the diamond lattice, highlighting the widespread nature of primary defect formation. Vacancy defects, along with $\langle 111 \rangle$ and $\langle 100 \rangle$ oriented dumbbell-shaped interstitial defects induced by high-dose neutron irradiation, were directly imaged, providing microscopic structural evidence that complements spectroscopic studies of point defects. Dynamical simulations combined with an adiabatic recombination-based damage model provided insights into the correlation between irradiation dose and resulting crystal damage. These findings advance our understanding of neutron-induced damage mechanisms in diamond and contribute to the development of radiation-resistant diamond materials.