The Influence of Crystal Anisotropy in Femtosecond Laser Processing of Single-Crystal Diamond.

The single-crystal diamond (SCD), owing to its extreme physical and chemical properties, serves as an ideal substrate for quantum sensing and high-frequency devices. However, crystal anisotropy imposes significant challenges on fabricating high-quality micro-nano structures, directly impacting device performance. This work investigates the effects of femtosecond laser processing on the SCD under two distinct crystallographic orientations via single-pulse ablation. The results reveal that ablation craters along the <100> orientation exhibit an elliptical shape with the major axis parallel to the laser polarization, whereas those along the <110> orientation form near-circular craters with the major axis at a 45° angle to the polarization. The single-pulse ablation threshold of the SCD along <110> is 9.56 J/cm, representing a 7.8% decrease compared to 10.32 J/cm for <100>. The graphitization threshold shows a more pronounced reduction, dropping from 4.79 J/cm to 3.31 J/cm (31% decrease), accompanied by enhanced sp carbon order evidenced by the significantly intensified G-band in the Raman spectra. In addition, a phase transition layer of amorphous carbon at the nanoscale in the surface layer (thickness of ~40 nm) and a narrow lattice spacing of 0.36 nm are observed under TEM, corresponding to the interlayer (002) plane of graphite. These observations are attributed to the orientation-dependent energy deposition efficiency. Based on these findings, an optimized crystallographic orientation selection strategy for femtosecond laser processing is proposed to improve the quality of functional micro-nano structures in the SCD.