Big-Data Reflection High Energy Electron Diffraction Analysis for Understanding Epitaxial Film Growth Processes

Reflection high energy electron diffraction (RHEED) has by now become a standard tool for in situ monitoring of film growth by pulsed laser deposition and molecular beam epitaxy. Yet despite the widespread adoption and wealth of information in RHEED images, most applications are limited to observing intensity oscillations of the specular spot, and much additional information on growth is discarded. With ease of data acquisition and increased computation speeds, statistical methods to rapidly mine the data set are now feasible. Here, we develop such an approach to the analysis of the fundamental growth processes through multivariate statistical analysis of a RHEED image sequence. This approach is illustrated for growth of LaxCa1-xMnO3 films grown on etched (001) SrTiO3 substrates, but is universal. The multivariate methods including principal component analysis and k-means clustering provide insight into the relevant behaviors, the timing and nature of a disordered to ordered growth change, and highlight statistically significant patterns. Fourier analysis yields the harmonic components of the signal and allows separation of the relevant components and baselines, isolating the asymmetric nature of the step density function and the transmission spots from the imperfect layer-by-layer (LBL) growth. These studies show the promise of big data approaches to obtaining more insight into film properties during and after epitaxial film growth. Furthermore, these studies open the pathway to use forward prediction methods to potentially allow significantly more control over growth process and hence final film quality.