π-Electronic Co-crystal Microcavities with Selective Vibronic-Mode Light Amplification: Toward Förster Resonance Energy Transfer Lasing
- Daichi OkadaDaichi OkadaDivision of Materials Science, Faculty of Pure and Applied Sciences, University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki 305-8573, JapanMore by Daichi Okada,
- Stefano AzziniStefano AzziniISIS & icFRC, Université de Strasbourg and CNRS, 8 allée Gaspard Monge, Strasbourg 67000, FranceMore by Stefano Azzini,
- Hiroki NishiokaHiroki NishiokaDepartment of Chemistry, The University of Tokyo, Hongo, Bunkyo-ku, Tokyo 113-0033, JapanMore by Hiroki Nishioka,
- Anna IchimuraAnna IchimuraDepartment of Chemistry, The University of Tokyo, Hongo, Bunkyo-ku, Tokyo 113-0033, JapanMore by Anna Ichimura,
- Hayato TsujiHayato TsujiDepartment of Chemistry, The University of Tokyo, Hongo, Bunkyo-ku, Tokyo 113-0033, JapanDepartment of Chemistry, Faculty of Science, Kanagawa University, 2946 Tsuchiya, Hiratsuka 259-1293, JapanMore by Hayato Tsuji,
- Eiichi NakamuraEiichi NakamuraDepartment of Chemistry, The University of Tokyo, Hongo, Bunkyo-ku, Tokyo 113-0033, JapanMore by Eiichi Nakamura,
- Fumio SasakiFumio SasakiElectronics and Photonics Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Umezono, Tsukuba, Ibaraki 305-8568, JapanMore by Fumio Sasaki,
- Cyriaque GenetCyriaque GenetISIS & icFRC, Université de Strasbourg and CNRS, 8 allée Gaspard Monge, Strasbourg 67000, FranceMore by Cyriaque Genet,
- Thomas W. EbbesenThomas W. EbbesenISIS & icFRC, Université de Strasbourg and CNRS, 8 allée Gaspard Monge, Strasbourg 67000, FranceMore by Thomas W. Ebbesen, and
- Yohei Yamamoto*Yohei Yamamoto*E-mail: [email protected]Division of Materials Science, Faculty of Pure and Applied Sciences, Tsukuba Research Center for Energy Materials Science (TREMS), , University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki 305-8573, JapanMore by Yohei Yamamoto
Abstract
π-conjugated organic microcrystals often act as optical resonators in which the generated photons in the crystal are confined by the reflection at the crystalline facets and interfere to gain lasing action. Here, we fabricate microcrystals from a mixture of carbon-bridged oligo-para-phenylenevinylenes (COPVs) with energy-donor (D) and energy-acceptor (A) characters. Upon weak excitation of the single D–A co-crystal, Förster resonance energy transfer (FRET) takes place, exhibiting spontaneous emission from A. In contrast, upon strong pumping, stimulated emission occurs before FRET, generating lasing action from D. Lasing occurs with single- and dual-vibronic levels, and the lasing wavelength can be modulated by the doping amount of A. Time-resolved spectroscopic studies reveal that the rate constant of lasing is more than 20 times greater than that of FRET. Furthermore, microcrystals, vertically grown on a Ag-coated substrate, reduce the lasing threshold by one-fourth. This study proposes possible directions toward organic solid FRET lasers with microcrystalline resonators.
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