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


Type
Article
Change log
Authors
Gu, Qinying 
Chotard, Florian 
Reponen, Antti-Pekka M  ORCID logo  https://orcid.org/0000-0002-2076-410X
Vitorica-Yrezabal, Inigo J 
Abstract

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 × 106 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.

Description

Funder: Samsung Display Corp.

Keywords
34 Chemical Sciences
Journal Title
Chem Mater
Conference Name
Journal ISSN
0897-4756
1520-5002
Volume Title
34
Publisher
American Chemical Society (ACS)
Sponsorship
Royal Society (RGF\EA\181008, URF\R1\180288, UF130278, RG140472)
Engineering and Physical Sciences Research Council (EP/M005143/1, EP/P012388/1, EP/R021503/1)
European Research Council (338944)