Hybridization of short-range and long-range charge transfer excited states in multiple resonance emitter

Ha Lim Lee, Jihoon Kang, Junseop Lim, Seung Chan Kim, Soon Ok Jeon () and Jun Yeob Lee ()
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Ha Lim Lee: Sungkyunkwan University 2066, Seobu-ro, Jangan-gu
Jihoon Kang: Sungkyunkwan University 2066, Seobu-ro, Jangan-gu
Junseop Lim: Sungkyunkwan University 2066, Seobu-ro, Jangan-gu
Seung Chan Kim: Sungkyunkwan University 2066, Seobu-ro, Jangan-gu
Soon Ok Jeon: Samsung Advanced Institute of Technology, Samsung Electronics, 130 Samsung-ro
Jun Yeob Lee: Sungkyunkwan University 2066, Seobu-ro, Jangan-gu

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: Abstract Multiple resonance (MR) thermally activated delayed fluorescence emitters have been actively studied as pure blue dopants for organic light-emitting diodes (OLEDs) because of excellent color purity and high efficiency. However, the reported MR emitter, 2,5,13,16-tetra-tert-butylindolo[3,2,1-jk]indolo[1′,2′,3′:1,7]indolo[2,3-b]carbazole (tDIDCz) based on bis-fused indolocarbazole framework could not demonstrate efficient triplet-to-singlet spin crossover. In this work, we report two isomeric MR emitters designed to promote triplet exciton harvesting by reconstructing the electronic structure of tDIDCz. To manage excited states, strong electron donors were introduced at the 2,5-/1,6-position of tDIDCz. As a result, 2,5-positions managed tDIDCz shows long-range charge transfer characteristics while preserving the MR nature. Quantum chemical calculation demonstrates direct spin-orbit coupling by long-range charge transfer and spin-vibronic coupling assisted reverse intersystem crossing by short-range charge transfer simultaneously contribute to triplet-to-singlet spin crossover. Consequently, high performance blue OLED recorded a high external quantum efficiency of 30.8% at a color coordinate of (0.13, 0.13).

Date: 2023
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DOI: 10.1038/s41467-023-40481-w

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