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Molecularly Dispersed Donors in Acceptor Molecular Crystals for Photon Upconversion under Low Excitation Intensity
Authors:Masanori Hosoyamada  Dr Nobuhiro Yanai  Taku Ogawa  Prof?Dr Nobuo Kimizuka
Affiliation:1. Department of Chemistry and Biochemistry, Graduate School of Engineering, Center for Molecular Systems (CMS), Kyushu University, Nishi-ku, Fukuoka, Japan;2. PRESTO, JST, Kawaguchi, Saitama, Japan
Abstract:For real‐world applications of photon upconversion based on the triplet–triplet annihilation (TTA‐UC), it is imperative to develop solid‐state TTA‐UC systems that work effectively under low excitation power comparable to solar irradiance. As an approach in this direction, aromatic crystals showing high triplet diffusivity are expected to serve as a useful platform. However, donor molecules inevitably tend to segregate from the host acceptor crystals, and this inhomogeneity results in the disappointing performance of crystalline state TTA‐UC. In this work, a series of cast‐film‐forming acceptors was developed, which provide both regular acceptor alignment and soft domains of alkyl chains that accommodate donor molecules without segregation. A typical triplet sensitizer, PtII octaethylporphyrin (PtOEP), was dispersed in these acceptor crystals without aggregation. As a result, efficient triplet energy transfer from the donor to the acceptor and diffusion of triplet excitons among regularly aligned anthracene chromophores occurred. It resulted in TTA‐UC emission at low excitation intensities, comparable to solar irradiance.
Keywords:crystal phases  photochemistry  photon upconversion  triplet energy migration  triplet–  triplet annihilation
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