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Plasma-enhanced atomic layer deposition (PEALD) enables the epitaxial growth of ultrathin indium nitride (InN) films at significantly reduced process temperatures and with greater control of layer thickness compared to other growth methods. However, the reliance on plasma-surface interactions increases the complexity of the growth process. A detailed understanding of the relationship between the plasma properties and the growth kinetics is therefore required to guide the tuning of growth parameters. We present an in situ investigation of the early-stage PEALD growth kinetics of epitaxial InN within three different plasma regimes using grazing incidence small-angle x-ray scattering (GISAXS). The GISAXS data are supported by diagnostic studies of the plasma species generation in the inductively coupled plasma source as a function of the relative concentrations of the nitrogen/argon gas mixture used in the growth process. The growth mode is found to be correlated to the production of nitrogen species in the plasma, with high concentrations of the atomic N species promoting Volmer–Weber growth (i.e., island growth) and low concentrations promoting Stranski–Krastanov growth (i.e., layer-plus-island growth). The critical thickness for island formation, island center-to-center distance, and island radius are found to increase with ion flux. Furthermore, the island center-to-center distance and areal density are observed to change only during plasma exposure and to continue changing with exposure even after the methylindium adlayer is believed to have fully reacted with the plasma. Our results demonstrate the potential to control the growth kinetics during PEALD of epitaxial films by intentionally accessing specific regimes of plasma species generation.

The properties of artificially grown thin films are strongly affected by surface processes during growth. Coherent X-rays provide an approach to better understand such processes and fluctuations far from equilibrium. Here we report results for vacuum deposition of C₆₀on a graphene-coated surface investigated with X-ray Photon Correlation Spectroscopy in surface-sensitive conditions. Step-flow is observed through measurement of the step-edge velocity in the late stages of growth after crystalline mounds have formed. We show that the step-edge velocity is coupled to the terrace length, and that there is a variation in the velocity from larger step spacing at the center of crystalline mounds to closely-spaced, more slowly propagating steps at their edges. The results extend theories of surface growth, since the behavior is consistent with surface evolution driven by processes that include surface diffusion, the motion of step-edges, and attachment at step edges with significant step-edge barriers.