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Sophisticated thin film growth techniques increasingly rely on the additionof a plasma component to open or widen a processing window, particularly at lowtemperatures. However, the addition of the plasma into the growth environmentalso complicates the surface dynamical evolution. Taking advantage of continuedincreases in accelerator-based X-ray source brilliance, this real-time studyuses X-ray Photon Correlation Spectroscopy (XPCS) to elucidate the nanoscalesurface dynamics during Plasma-Enhanced Atomic Layer Deposition (PE-ALD) of anepitaxial indium nitride film. XPCS examines the evolution of the coherentX-ray scattering speckle pattern, which is a fingerprint of the unique samplemicrostructure at each moment in time. In PE-ALD, ultrathin films aresynthesized from repeated cycles of alternating self-limited surface reactionsinduced by temporally-separated pulses of material precursor and plasmareactant, allowing the influence of each on the evolving morphology to beexamined. During the heteroepitaxial 3D growth examined here, sudden changes insurface structure during initial film growth, consistent with numerousoverlapping stress-relief events, are observed. When the film becomescontinuous, the nanoscale surface morphology abruptly becomes long-lived withcorrelation time spanning the period of the experiment. Throughout the growthexperiment, there is a consistent repeating pattern of correlations associatedwith the cyclic growth process, which is modeled as transitions betweendifferent surface states. The plasma exposure does not simply freeze in astructure that is then built upon in subsequent cycles, but rather there isconsiderable surface evolution during all phases of the growth cycle.

Coherent X-ray Spectroscopy Elucidates Nanoscale Dynamics of Plasma-Enhanced Thin-Film Growth