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Improved Surface Passivation of Colloidal Ge1–xSnx Nanoalloys through Amorphous SiO2 Shell Growth

MetadataDetails
Publication Date2022-06-02
JournalThe Journal of Physical Chemistry C
AuthorsDrew Z. Spera, Indika U. Arachchige
InstitutionsVirginia Commonwealth University
Citations8

Ge1-xSnx alloy nanocrystals (NCs) are a class of semiconductors that show interesting (photo)physical properties such as composition-dependent visible to near-IR energy gaps and enhanced light-matter interactions compared to single element Ge NCs. With decreasing size and increasing Sn content, the molar absorptivity and emission efficiency increase, making these NCs attractive for optoelectronic, molecular imaging, and sensing studies. To further improve the optical stability, there is a need to passivate the Ge1-xSnx surface with a robust shell material to protect the core from oxidation and inhibit chemical exchange when exposed to extreme environments. Herein, we report a fluent synthetic method for the growth of a thin silica layer on bulk-like (14.9 ± 1.7 nm) and quantum-confined (4.4 ± 0.6 nm) Ge1-xSnx NCs. Physical characterization of Ge1-xSnx/SiO2 core/shell NCs suggests that the diamond cubic structure of the core is retained upon shell growth, whereas solid-state and solution-state absorption spectra confirm the composition-dependent energy gap tunability. The core-shell NCs (1.23-2.07 eV for x = 0.03-0.09) show an average energy gap increase of 0.38 eV relative to the core NCs (0.91-1.67 eV for x = 0.03-0.09) owing to minor surface etching induced by shell growth. Surface analysis of core-shell NCs suggests a notable decrease in Ge2+ species and greater dominance of Ge0 species relative to the organically passivated Ge1-xSnx core NCs, confirming the production of robust, oxidation-resistant, and optically stable Ge1-xSnx/SiO2 alloy NCs.