“…Since early demonstrations of femtosecond laser as a three-dimensional (3D) processing tool, [1][2][3][4] microdevices with exciting optical, electronic, mechanical, and magnetic functions have been manufactured, [5][6][7][8][9] by which novel concepts from 3D quantum photonic integrated circuits to intelligent micro-robots are enabled. [10][11][12] Much effort in the past decade in this eld has been devoted to improving manufacture resolution, and several tens of nanometer feature sizes, far beyond the optical diffraction limit, have been reported based on multiphoton absorption, 1 stimulation emission depletion, 13,14 fareld-induced near-eld enhancement, 15 and photoexcitation-induced chemical bonding effects. 16 Nevertheless, singleelectron transistors, single-photon emitters, single-atom memory, and quantum-bit devices require higher manufacturing accuracy, i.g., the ability to address single-atom defects complex (SADC) for initiating functions such as single-photon emission, as is still missing.…”