Abstract Two-photon etching of diamond surfaces is a novel technique for providing controlled removal of atomic layers and nano-patterning the surface. However, the details of the etching mechanism and pattern development are not well understood so that the full capability of the process is unclear. Here, a comprehensive investigation into the dynamics of nanopattern formation on the (100), (110) and (111) facets is reported as a function of polarization, for CVD and HPHT diamond, and for nanosecond and picosecond laser pulse durations. A diverse array of behaviour is observed including sub-wavelength scale structuring with morphologies characteristic of the facet and the selected polarization. As etching proceeds, the anisotropies in the quantum photon-lattice interaction are imprinted on the emergent patterns on nano and mesoscopic scales. The sum of the results leads to rules for predicting pattern type, roughness and etch rate. We also argue that they support a mechanism for carbon ejection based on the photo-ejection of carbonyl groups from carbonyl-supporting surfaces, defects and atomic-level step edges. The results provide guidance for optically manipulating diamond surfaces and comprise a major step towards a complete model for the process to aid laser direct-write structuring of functional diamond surfaces.

中文翻译：

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金刚石偏振双光子蚀刻形成的细观表面图案的形态发生

摘要 金刚石表面的双光子蚀刻是一种新技术，用于提供可控的原子层去除和表面纳米图案化。然而，蚀刻机制和图案开发的细节尚不清楚，因此该工艺的全部能力尚不清楚。在这里，对 (100)、(110) 和 (111) 小面上纳米图案形成的动力学进行了全面调查，作为极化的函数，对于 CVD 和 HPHT 金刚石，以及纳秒和皮秒激光脉冲持续时间。观察到一系列不同的行为，包括具有小平面和选定偏振特征的形态特征的亚波长尺度结构。随着蚀刻的进行，量子光子-晶格相互作用中的各向异性被印在纳米和介观尺度上的涌现图案上。结果的总和导致预测图案类型、粗糙度和蚀刻速率的规则。我们还认为，它们支持基于羰基从羰基支撑表面、缺陷和原子级台阶边缘光喷射出的碳喷射机制。结果为光学操作金刚石表面提供了指导，并且是朝着完整的过程模型迈出的重要一步，以帮助功能性金刚石表面的激光直写结构。