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Rutile GeO2 has been predicted to be an ultra-wide bandgap semiconductorsuitable for future power electronics devices while quartz-like GeO2 showspiezoelectric properties. To explore these crystalline phases for applicationand fundamental materials investigations, molecular beam epitaxy (MBE) is awell-suited thin film growth technique. In this study, we investigate thereaction kinetics of GeO2 during plasma-assisted MBE using elemental Ge andplasma-activated oxygen fluxes. The growth rate as a function of oxygen flux ismeasured in-situ by laser reflectometry at different growth temperatures. Aflux of the suboxide GeO desorbing off the growth surface is identified andquantified in-situ by the line-of-sight quadrupole mass spectrometry. Ourmeasurements reveal that the suboxide formation and desorption limits thegrowth rate under metal-rich or high temperature growth conditions, and leadsto etching of the grown GeO2 layer under Ge flux in the absence of oxygen. Thequantitative results fit the sub-compound mediated reaction model, indicatingthe intermediate formation of the suboxide at the growth front. This model isfurther utilized to delineate the GeO2-growth window in terms of oxygen-fluxand substrate temperature. Our study can serve as a guidance for the thin filmsynthesis of GeO2 and defect-free mesa etching in future GeO2-deviceprocessing.

In-situ study and modeling of the reaction kinetics during molecular beam epitaxy of GeO2 and its etching by Ge