Low-Cost Synthesis of Silicon Quantum Dots with Near-Unity Internal Quantum Efficiency

J Phys Chem Lett. 2021 Sep 23;12(37):8909-8916. doi: 10.1021/acs.jpclett.1c02187. Epub 2021 Sep 9.

Abstract

As a cost-effective batch synthesis method, Si quantum dots (QDs) with near-infrared photoluminescence, high quantum yield (>50% in polymer nanocomposite), and near-unity internal quantum efficiency were fabricated from an inexpensive commercial precursor (triethoxysilane, TES), using optimized annealing and etching processes. The optical properties of such QDs are similar to those prepared from state-of-the-art precursors (hydrogen silsesquioxane, HSQ) yet featuring an order of magnitude lower cost. To understand the effect of synthesis parameters on QD optical properties, we conducted a thorough comparison study between common solid precursors: TES, HSQ, and silicon monoxide (SiO), including chemical, structural, and optical characterizations. We found that the structural nonuniformity and abundance of oxide inherent to SiO limited the resultant QD performance, while for TES-derived QDs this drawback can be avoided. The presented low-cost synthetic approach would significantly favor applications requiring high loading of good-quality Si QDs, such as light conversion for photovoltaics.