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Emerging two-dimensional gallium chalcogenides, such as gallium telluride (GaTe), are considered promising layered semiconductors that can serve as vital building blocks towards the implementation of nanodevices in the fields of nanoelectronics, optoelectronics, and quantum photonics. However, oxidation-induced electronic, structural, and optical changes observed in ambient-exposed gallium chalcogenides need to be further investigated and addressed. Herein, we report on the thickness-dependent effect of air exposure on the Raman and photoluminescence (PL) properties of GaTe flakes, with thicknesses spanning in the range of a few layers to 100 nm. We have developed a novel chemical passivation that results in complete encapsulation of the as-exfoliated GaTe flakes in ultrathin hydrogen−silsesquioxane (HSQ) film. A combination of correlation and comparison of Raman and PL studies reveal that the HSQ-capped GaTe flakes are effectively protected from oxidation in air ambient over the studied-period of one year, and thus, preserving their structural and optical characteristics. This contrasts with the behavior of uncapped GaTe, where we observe a significant reduction of the GaTe-related PL (~100×) and Raman (~4×) peak intensities for the few-layered flakes over a period of few days. The time-evolution of the Raman spectra in uncapped GaTe is accompanied by the appearance of two new prominent broad peaks at ~130 cm−1 and ~146 cm−1, which are attributed to the formation of polycrystalline tellurium, due to oxidation of ambient-exposed GaTe. Furthermore, and by leveraging this novel passivation, we were able to explore the optical anisotropy of HSQ-capped GaTe flakes. This is caused by the one-dimensional-like nature of the GaTe layer, as the layer comprises Ga−Ga chains extending along the b-axis direction. In concurrence with high-resolution transmission electron microscopy analysis, polarization-dependent PL spectroscopy was used to identify the b-axis crystal direction in HSQ-capped GaTe flakes with various thicknesses over a range of wavelengths (458 nm−633 nm). Thus, our novel surface-passivation offers a new approach to explore and reveal the physical properties of the layered GaTe, with the potential of fabricating reliable polarization-dependent nanophotonics with structural and optical stability. |
