Al2O3 thin films were deposited by plasma enhanced atomic layer deposition (PEALD) from trimethylaluminum precursor and oxygen plasma at 250 °C on AlGaN/GaN heterostructures. Before deposition, the sample surfaces were treated with the following solutions: (A) H2O2:H2SO4 (piranha), (B) fluoride acid (HF) + HCl, and (C) piranha + HF for 10 min each. Transmission electron microscopy analysis revealed that, independently from the surface preparation, all the films are adherent and uniform with thicknesses of about 27–28 nm. However, a different structural evolution has been observed under electron beam effect. In particular, while all the as-deposited films were found to be amorphous, the formation of polycrystalline grains was observed on the sample deposited after the A treatment. On the other hand, oriented layers were formed on the samples deposited after B and C treatments. This result is an …