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Unusual Optical, Electric, and Magnetic Behaviors of OLEDs due to Exothermic/Endothermic Dexter-Energy-Transfer and Fusion Channels of Hot/Cold Triplet Excitons
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    Unusual Optical, Electric, and Magnetic Behaviors of OLEDs due to Exothermic/Endothermic Dexter-Energy-Transfer and Fusion Channels of Hot/Cold Triplet Excitons
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    • Yuting Wu
      Yuting Wu
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
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    • Jingjing Wang
      Jingjing Wang
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
    • Jing Chen
      Jing Chen
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
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    • Huiyao Wang
      Huiyao Wang
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
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    • Song Yang
      Song Yang
      School of Science, Guizhou University of Engineering Science, Bijie 551700, China
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    • Hong Lu
      Hong Lu
      School of Science, Guizhou University of Engineering Science, Bijie 551700, China
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    • Junhong Liu
      Junhong Liu
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
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    • Bo Wang
      Bo Wang
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
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    • Teng Peng
      Teng Peng
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
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    • Jun Yang
      Jun Yang
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
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    • Yingqiong Zhou
      Yingqiong Zhou
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
    • Keyi Zhang
      Keyi Zhang
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
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    • Zuo Li
      Zuo Li
      School of Science, Guizhou University of Engineering Science, Bijie 551700, China
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    • Yingfei Yi
      Yingfei Yi
      School of Science, Guizhou University of Engineering Science, Bijie 551700, China
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    • Lihong Cheng
      Lihong Cheng
      School of Science, Guizhou University of Engineering Science, Bijie 551700, China
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    • Sijie Zhang*
      Sijie Zhang
      School of Science, Guizhou University of Engineering Science, Bijie 551700, China
      College of Physics, Sichuan University, Chengdu 610065, China
      *Email: [email protected]
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    • Tian Yu
      Tian Yu
      College of Physics, Sichuan University, Chengdu 610065, China
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    • Hongqiang Zhu
      Hongqiang Zhu
      Chongqing Key Laboratory of Photo-Electric Functional Materials, Chongqing Normal University, Chongqing 401331, China
    • Zuhong Xiong*
      Zuhong Xiong
      Chongqing Key Laboratory of Micro&Nano Structure Optoelectronics, School of Physical Science and Technology, Southwest University, Chongqing 400715, China
      *Email: [email protected]
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    ACS Photonics

    Cite this: ACS Photonics 2024, 11, 11, 4567–4577
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    https://doi.org/10.1021/acsphotonics.4c00809
    Published November 1, 2024
    Copyright © 2024 American Chemical Society

    Abstract

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    Hot-exciton-based organic light-emitting diodes (HE-OLEDs) have aroused more attention due to their advantages of low cost, high efficiency, and negligible efficiency roll-off. However, their physical behaviors need further investigation because of the evolution diversity of excited states existing in HE-OLEDs. Herein, we employ the two frequently used hosts tris(8-hydroxyquinoline)aluminum (Alq3) and 4,4′-N,N′-dicarbazolebiphenyl (CBP) and the hot-exciton emissive guests rubrene (Rb) and its derivative 2,8-di-tert-butyl-5,11-bis(4-tert-butylphenyl)-6,12-diphenyltetracene (TBRb) to make four HE-OLEDs and use well-known fingerprint magneto-electroluminescence (MEL) curves to probe their microscopic dynamic processes. Interestingly, we find abundant optical, electric, and magnetic behaviors of HE-OLEDs due to exothermic and endothermic Dexter-energy-transfer (DET) and triplet fusion (TF) channels of hot/cold excitons. Specifically, for the case of different bias currents at room temperature, both the low-field MEL curves of Rb- and TBRb-doped Alq3-based OLEDs show a normal intersystem crossing (ISC) of polaron pairs, but those of Rb- and TBRb-doped CBP-based OLEDs present a conversion from a high-level reverse ISC (HL-RISC, S1 ← T2) to an ISC and a normal HL-RISC, respectively, which weakens with an elevated bias current. Moreover, both the high-field MEL curves of Rb- and TBRb-doped Alq3-based (CBP-based) OLEDs show a normal T1F (T2F) of cold (hot) triplet excitons, which strengthens with elevated bias currents. For the case of constant bias currents at variable temperatures, both the low-field MEL curves of Rb- and TBRb-doped Alq3-based OLEDs show an abnormal ISC, which rises with a reducing temperature, but those of Rb- and TBRb-doped CBP-based OLEDs depict a conversion from an ISC to a HL-RISC and a normal HL-RISC, respectively, which intensifies with a decreasing temperature. In addition, the high-field MEL curves of Rb- and TBRb-doped Alq3-based OLEDs separately show a normal and an abnormal T1F, but those of both of Rb- and TBRb-doped CBP-based OLEDs exhibit a normal T2F, which strengthens with a reducing temperature. Furthermore, the quantum efficiency of Rb- and TBRb-doped Alq3-based OLEDs separately show nonmonotonically and monotonically decreased tendencies, but both Rb- and TBRb-doped CBP-based OLEDs show monotonically increased tendencies with a decreasing temperature. Surprisingly, all of the above enriched physical behaviors can be reasonably interpreted within the frames of excited state dynamics that DET from host cold T1,Alq3 (T1,CBP) to guest hot T2 is an endothermic (exothermic) process and T1F in Rb (TBRb) is an exothermic (endothermic) process, but T2F in both Rb and TBRb is exothermic.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsphotonics.4c00809.

    • Quantitative discussion of a guest’s molar absorption coefficients for determining FRET rates from hosts Alq3 and CBP to guests Rb andt TBRb; specific reasons for ignoring DCI effects in devices 1–4 with a low guest concentration of 2%; relationships between luminescence and current and between the slope of the LI line and luminous quantum efficiency; summaries of energy levels and singlet and triplet energies of the materials; optoelectronic performance data and characteristics of devices 1–4; characteristic MEL curves of B-mediated ISC, RISC, TF, and SF processes; molecular structures of Alq3, CBP, Rb, and TBRb; cartoon configurations of the prepared devices; current- and temperature-dependent MEL curves in a small range of B (|B| ≤ 30 mT) from devices 1–4; normalized EL spectra of devices 2 and 2A–2D and devices 4 and 4A–4D; concentration-dependent MEL curves in a small range of B (|B| ≤ 30 mT) from devices 2 and 4; MEL comparisons and EQE–L characteristics of devices 1 and 1A and devices 3 and 3A under a bias current of 100 μA (PDF)

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    ACS Photonics

    Cite this: ACS Photonics 2024, 11, 11, 4567–4577
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsphotonics.4c00809
    Published November 1, 2024
    Copyright © 2024 American Chemical Society

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