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  1. Free, publicly-accessible full text available August 1, 2024
  2. Photon upconversion in systems incorporating inorganic quantum dots (QDs) is of great interest for applications in solar energy conversion, bioimaging, and photodynamic therapy. Achieving high up-conversion efficiency requires not only high-quality inorganic nanoparticles, but also precise control of their surface functional groups. Gas-phase surface functionalization provides a new pathway towards controlling the surface of small inorganic nanoparticles. In this contribution, we utilize a one-step low-temperature plasma technique for the synthesis and in-flight partial functionalization of silicon QDs with alkyl chains. The partially functionalized surface is then modified further with 9-vinylanthracene via thermal hydrosilylation resulting in the grafting of 9-ethylanthracene (9EA) groups. We have found that the minimum alkyl ligand density necessary for quantum dot solubility also gives the maximum upconversion quantum yield, reaching 17% for silicon QDs with Si-dodecyl chains and an average of 3 9EA molecules per particle. 
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  4. Abstract

    Photon upconversion may have the highest impact in biological applications because incoming photons transparent to tissue can be combined to make visible light useful for photodynamic therapy and imaging. The ability to use semiconductor nanocrystals as light absorbers for photon upconversion is important because their strong absorption profiles are synthetically tunable. In particular, the use of earth‐abundant, environmentally benign silicon quantum dots (QDs) as light absorbers for photon upconversion is very attractive. In this work, the authors demonstrate a general strategy employing both physical and chemical barriers to achieve air‐stable fusion of triplet excitons photosensitized by silicon QDs, crucial to practical applications of photon upconversion. Gel permeation chromatography (GPC) and dynamic light scattering (DLS) show that thermal hydrosilylation critical for colloidal stability and efficient triplet energy transfer creates a polymeric barrier to oxygen. This kinetic barrier to oxygen arises from the presence of cross‐linked surfactants and is complemented by the sacrificial oxidation of silicon QDs itself. Photon upconversion lasted longer than 4 days with quantum yields (QYs) as high as 7.5% (out of a maximum of 50%) using Si QD light absorbers with diphenylanthracene in methyl oleate. Oil‐in‐water micelles are air‐stable for 2 days with absolute upconversion QYs of 5.5%.

     
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