Reducing dislocation defect levels via sub-melt nanosecond pulsed-laser induced densification of diamond

Abstract: Dislocations and polishing-induced defect networks in synthetic diamond generate local strain fields that broaden Raman features and limit optical, thermal, and electronic performance. Sub-melt laser annealing has emerged as a route to repair near-surface defects without graphitization, yet quantitative evidence of densification, defect depletion, and property recovery remains limited. Here, we show that nanosecond pulsed-laser annealing (PLA) can relax dislocation-associated strain in single-crystal CVD diamond by compacting and reorganizing the damaged near-surface region. Single- and two-pulse PLA were applied, and structural evolution was quantified using co-registered ISO 25178 white-light interferometry, depth-resolved Raman spectroscopy, and cross-sectional STEM with geometric phase analysis (GPA). Across a 5x6 grid(n = 30), responsive regions show large reductions in local slope (Sdq 45-65%), developed area (Sdr 60-90%), height spread (Sp, Sz 30-65%), void volume (Vv 57-60%), and roughness amplitude (Sa, Sq 48-57%), consistent with densification of ~4-6.5 nm. Raman profiling reveals narrowing of the diamond line and improved spectral uniformity to depths of ~2-3 μm, indicating relaxation of dislocation-mediated strain beyond the compaction layer. STEM-GPA strain maps confirm smoother strain fields, reduced hotspots, and redistribution of localized strain concentrations after PLA. These results show that sub-melt PLA reduces dislocation-driven strain by compacting surface-connected free volume and reorganizing defect networks. The approach provides a scalable path to upgrade industrial-grade diamond including homoepitaxial, heteroepitaxial, and polycrystalline CVD to low-defect, device-ready surfaces relevant to high-power electronics, photonics, and quantum substrates.