An ALE system for performing a metal ALE process to etch a surface of a substrate includes a processing chamber, a substrate support, a heat source, a delivery system, and a controller. The substrate support is disposed in the processing chamber and supports the substrate. The delivery system supplies a ligand or organic species to the processing chamber. The controller controls the delivery system and the heat source to perform an isotropic metal ALE process that includes: during an iteration of the isotropic metal ALE process, performing atomistic adsorption and pulsed thermal annealing; during the atomistic adsorption, exposing the surface to the ligand or organic species, where the ligand or organic species is void of a metal precursor and is selectively adsorbed to form a metal complex in the surface; and during the pulsed thermal annealing, pulsing the heat source multiple times to remove the metal complex from the substrate.