In-cycle evolution of thickness and roughness parameters during oxygen plasma enhanced ZnO atomic layer deposition using <i>in situ</i> spectroscopic ellipsometry

We investigate the time evolution of ZnO thin film growth in oxygen plasma-enhanced atomic layer deposition using in situ spectroscopic ellipsometry. The recently proposed dynamic-dual-box-model approach [Kilic et al., Sci. Rep. 10, 10392 (2020)] is used to analyze the spectroscopic data post-growth. With the help of this model, we explore the in-cycle surface modifications and reveal the repetitive layer-by-layer growth and surface roughness modification mechanisms during the ZnO ultrathin film deposition. The in situ complex-valued dielectric function of the amorphous ZnO thin film is also determined from the model analysis for photon energies of 1.7–4 eV. The dielectric function is analyzed using a critical point model approach providing parameters for bandgap energy, amplitude, and broadening in addition to the index of refraction and extinction coefficient. The dynamic-dual-box-model analysis reveals the initial nucleation phase where the surface roughness changes due to nucleation and island growth prior to film coalescence, which then lead to the surface conformal layer-by-layer growth with constant surface roughness. The thickness evolution is resolved with Angstrom-scale resolution vs time. We propose this method for fast development of growth recipes from real-time in situ data analysis. We also present and discuss results from x-ray diffraction, x-ray photoelectron spectroscopy, and atomic force microscopy to examine crystallographic, chemical, and morphological characteristics of the ZnO film.