Title: Treatment and Aging Studies of GaAs(111)B Substrates for van der Waals Chalcogenide Film Growth

Abstract: GaAs(111)B is a semiconductor substrate widely used in research and commercial fields due to its low cost, mature synthesis technology, and excellent properties for manufacturing electronic devices. It is not only used to grow three-dimensional (3D) strongly-bonded materials, but has also been used as a substrate for layered, van der Waals (vdW)-bonded chalcogenide film growth. However, GaAs(111)B wafers cannot be directly used for growing epitaxial vdW chalcogenide films for two reasons: (1) the GaAs surface has a substantial number of dangling bonds that need to be passivated for vdW layers growth; (2) the substrate surface is covered with a thin epi-ready oxide layer which must be removed before film growth. In this paper, we optimize the method for deoxidizing GaAs(111)B substrates under a Se overpressure and successfully create a smooth, deoxidized, and passivated substrate for subsequent growth of vdW chalcogenide materials. We demonstrate the benefits of this method for the growth of vdW chalcogenide thin films using GaSe as a representative of vdW chalcogenides. In addition, we find that severely aged substrates have difficulty maintaining a smooth surface during the deoxidation and passivation process and cause GaSe crystals to nucleate in random shapes and orientations. We describe a method using water droplet testing to determine the age of the substrate. Finally, X-ray photoelectron spectroscopy (XPS) characterization reveals that the natural aging of GaAs(111)B in the air results in an increase in surface oxides, Ga2O3 and As2O3, while exposure to ultraviolet (UV)-ozone not only enhances the contents of these two oxides but also generates a new oxide, As2O5. Our research contributes to expanding the compatibility of GaAs(111)B with diverse growth materials and the production of high-quality heterostructure devices.