Ion beams of sufficient energy to erode a surface can lead to surface modulations that depend on the ion beam, the material surface it impinges, and extrinsic parameters such as temperature and geometric boundary conditions. Focused Ion Beam technology both enables site-specific placement of these modulations and expedites research through fast, high dose and small efficient use of material. The DualBeam (FIB/SEM) enables in situ metrology, with movies observing ripple formation, wave motion, and the influence of line defects. Nanostructures (ripples of >400nm wavelength to dots spaced <40nm) naturally grow from atomically flat surfaces during erosion, however, a steady state size may or may not be achieved as a consequence of numerous controlled parameters: temperature, angle, energy, crystallography. Geometric factors, which can be easily invoked using a FIB, enable a controlled component of deposition (and/or redeposition) to occur during erosion, and conversely allow a component of etching to be incurred during (ion-beam assisted) deposition. High angles of ion beam inclination commonly lead to “rougher” surfaces, however, the extreme case of 90.0° etching enables deposition of organized structures 1000 times smaller than the aforementioned, video-recorded nanostructures. Orientation and position of these picostructures (naturally quantized by their atomic spacings) may be controlled by the same parameters as for nanostructures (e.g. ion inclination and imposed boundary conditions, which are flexibly regulated by FIB). Judicious control of angles during FIB-CVD growth stimulates erosion with directionality that produces surface modulations akin to those observed for sputtering. Just as a diamond surface roughens from 1-D ripples to 2-D steps with increasing angle of ion sputtering, so do ripples and steps appear on carbon-grown surfaces with increase in angle of FIB-CVD. Ion beam processing has been a stalwart of the microelectronics industry, is now a vital tool for research of self-organizing nanostructures, and promises to be a focus for future picotechnology.