van der Waals solid solution crystals for highly efficient in-air photon upconversion under subsolar irradiance

Riku Enomoto; Megumi Hoshi; Hironaga Oyama; Hideki Agata; Shinichi Kurokawa; Hitoshi Kuma; Hidehiro Uekusa; Yoichi Murakami

doi:10.1039/D1MH01542G

van der Waals solid solution crystals for highly efficient in-air photon upconversion under subsolar irradiance†

Riku Enomoto,

^a Megumi Hoshi,^a Hironaga Oyama,^b Hideki Agata,^c Shinichi Kurokawa,^d Hitoshi Kuma,^d Hidehiro Uekusa^b and Yoichi Murakami

*^ae

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* Corresponding authors

^a School of Engineering, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo 152-8552, Japan
E-mail: murakami.y.af@m.titech.ac.jp

^b Department of Chemistry, Tokyo Institute of Technology, 2-12-1 Ookayama, Meguro-ku, Tokyo 152-8551, Japan

^c Nissan Motor Co., Ltd., 2 Takaracho, Kanagawa-ku, Yokohama, Kanagawa 220-8623, Japan

^d Idemitsu Kosan Co., Ltd., 1-2-1 Otemachi, Chiyoda-ku, Tokyo 100-8321, Japan

^e PRESTO, JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan

Abstract

Triplet-sensitized photon upconversion (UC) has been proposed for broad applications. However, the quest for superior solid materials has been challenged by the poor exciton transport often caused by low crystallinity, a small crystal domain, and aggregation of triplet sensitizers. Here, we demonstrate substantial advantages of the van der Waals solid solution concept to yield molecular crystals with extraordinary performance. A 0.001%-order porphyrin sensitizer is dissolved during recrystallization into the molecular crystals of a blue-fluorescent hydrocarbon annihilator, 9-(2-naphthyl)-10-[4-(1-naphthyl)phenyl]anthracene (ANNP), which contains bulky side groups. This attempt yields millimeter-sized, uniformly colored, transparent solid solution crystals, which resolves the long-standing problem of sensitizer aggregation. After annealing, the crystals exhibit unprecedented UC performance (UC quantum yield reaching 16% out of a maximum of 50% by definition; excitation intensity threshold of 0.175 sun; and high photostability of over 150 000 s) in air, which proves that this concept is highly effective in the quest for superior UC solid materials.

This article is part of the themed collections: 2021 Horizons Outstanding Paper Award Winners and Materials Horizons Lunar New Year collection 2022

Materials Horizons

van der Waals solid solution crystals for highly efficient in-air photon upconversion under subsolar irradiance†

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van der Waals solid solution crystals for highly efficient in-air photon upconversion under subsolar irradiance

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