Solid-state sensitized liquid-chromophore triplet fusion upconversion

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Abstract
Photochemical upconversion has several potential applications in optoelectronics. However, there is yet to be demonstrated a rational approach to high efficiencies in nanoscale solid state devices. Here we demonstrate that the liquid triplet fusion medium, 9,10-bis(n-octyl-diisopropylsilylethynyl)anthracene (NODIPS-An), which behaves as a solid on excitonic time-scales, can achieve high efficiency upconversion on the nanoscale. Due to its amorphous structure, there are highly-coupled sites that trap upconverted states and prevent the back-transfer that plagues nanoscale upconversion systems. With NODIPS-An filling the pores of a sensitized alumina nano-scaffold, we achieve an absolute photon upconversion efficiency of 7.0%. The efficiency losses are entirely attributed to fluorescence yield and triplet energy transfer, and thus the self-trapping of excitons within the triplet fusion medium is demonstrated to effectively prevent the back transfer of excitons to the sensitizer. Strategies are proposed to improve the fluorescence yield and triplet energy transfer to pursue higher efficiencies in nanoscale solid-state photochemical upconversion devices.
Funding Information
  • Centre of Excellence in Exciton Science (CE170100026)
  • Australian Research Council (FT230100002)
  • Australian Research Council (DE230100382)

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