4.8 Article

Excited-State Lifetime Modulation by Twisted and Tilted Molecular Design in Carbene-Metal-Amide Photoemitters

期刊

CHEMISTRY OF MATERIALS
卷 34, 期 16, 页码 7526-7542

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.2c01938

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资金

  1. Engineering and Physical Sciences Research Council (EPSRC) [EP/M005143/1, EP/R021503/1, EP/P012388/1]
  2. Royal Society [URF\R1\180288, RGF\EA\181008, UF130278, RG140472]
  3. European Research Council (ERC)
  4. Samsung Display Corp. (SDC)
  5. ERC Advanced Investigator Award [338944-GOCAT]

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Carbene-metal-amides (CMAs) are a new class of photoemitters with flexible conformations that significantly influence their photophysical properties. This study investigates four different conformations and their impact on luminescence efficiency and lifetime. Results show that partially twisted and/or tilted structures exhibit the highest performance. Additionally, proof-of-concept organic light-emitting diodes (OLEDs) based on these emitters were successfully fabricated.
Carbene-metal-amides (CMAs) are an emerging class of photoemitters based on a linear donor-linker-acceptor arrangement. They exhibit high flexibility about the carbene-metal and metal-amide bonds, leading to a conformational freedom which has a strong influence on their photophysical properties. Herein we report CMA complexes with (1) nearly coplanar, (2) twisted, (3) tilted, and (4) tilt-twisted orientations between donor and acceptor ligands and illustrate the influence of preferred ground-state conformations on both the luminescence quantum yields and excited-state lifetimes. The performance is found to be optimum for structures with partially twisted and/or tilted conformations, resulting in radiative rates exceeding 1 X 10(6) s(-1). Although the metal atoms make only small contributions to HOMOs and LUMOs, they provide sufficient spin-orbit coupling between the low-lying excited states to reduce the excited-state lifetimes down to 500 ns. At the same time, high photoluminescence quantum yields are maintained for a strongly tilted emitter in a host matrix. Proof-of-concept organic light-emitting diodes (OLEDs) based on these new emitter designs were fabricated, with a maximum external quantum efficiency (EQE) of 19.1% with low device roll-off efficiency. Transient electroluminescence studies indicate that molecular design concepts for new CMA emitters can be successfully translated into the OLED device.

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