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Atomic force microscopy (AFM)-based electrochemical etching of a highly oriented pyrolytic graphite (HOPG) surface is studied toward the single-atomic-layer lithography of intricate patterns. Electrochemical etching is performed in the water meniscus formed between the AFM tip apex and HOPG surface due to a capillary effect under controlled high relative humidity (~ 75%) at otherwise ambient conditions. The conditions to etch nano-holes, nano-lines, and other intricate patterns are investigated. The electrochemical reactions of HOPG etching should not generate debris due to the conversion of graphite to gaseous CO and CO₂ based on etching reactions. However, debris is observed on the etched HOPG surface, and incomplete gasification of carbon occurs during the etching process, resulting in the generation of solid intermediates. Moreover, the applied potential is of critical importance for precise etching …