Coherent X-ray spectroscopy reveals the persistence of island arrangements during layer-by-layer growth

Understanding surface dynamics during epitaxial film growth is key to growing high-quality materials with controllable properties. X-ray photon correlation spectroscopy (XPCS) using coherent X-rays opens new opportunities for in situ observation of atomic-scale fluctuation dynamics during crystal growth. Here, we present XPCS measurements of two-dimensional island dynamics during homoepitaxial growth in the layer-by-layer mode. Analysis of the results using two-time correlations reveals a new phenomenon—a memory effect in the arrangement of islands formed on successive crystal layers. Simulations indicate that this persistence in the island arrangements arises from communication between islands on different layers via adatoms. With the worldwide advent of new coherent X-ray sources, the experimental and analysis methods pioneered here will enable broad application of XPCS to observe atomic-scale processes on surfaces.