Achieving spin-triplet exciton transfer between silicon and molecular acceptors for photon upconversion.
Published Web Locationhttps://doi.org/10.1038/s41557-019-0385-8
Inorganic semiconductor nanocrystals interfaced with spin-triplet exciton-accepting organic molecules have emerged as promising materials for converting incoherent long-wavelength light into the visible range. However, these materials to date have made exclusive use of nanocrystals containing toxic elements, precluding their use in biological or environmentally sensitive applications. Here, we address this challenge by chemically functionalizing non-toxic silicon nanocrystals with triplet-accepting anthracene ligands. Photoexciting these structures drives spin-triplet exciton transfer from silicon to anthracene through a single 15 ns Dexter energy transfer step with a nearly 50% yield. When paired with 9,10-diphenylanthracene emitters, these particles readily upconvert 488-640 nm photons to 425 nm violet light with efficiencies as high as 7 ± 0.9% and can be readily incorporated into aqueous micelles for biological use. Our demonstration of spin-triplet exciton transfer from silicon to molecular triplet acceptors can critically enable new technologies for solar energy conversion, quantum information and near-infrared driven photocatalysis.