Donor N-Substitution as Design Principle for Fast and Blue Luminescence in Carbene-Metal-Amides
Authors
Reponen, APM
Chotard, F
Lempelto, A
Shekhovtsev, V
Credgington, D
Bochmann, M
Linnolahti, M
Greenham, NC
Publication Date
2022Journal Title
Advanced Optical Materials
ISSN
2195-1071
Publisher
Wiley
Language
en
Type
Article
This Version
AO
VoR
Metadata
Show full item recordCitation
Reponen, A., Chotard, F., Lempelto, A., Shekhovtsev, V., Credgington, D., Bochmann, M., Linnolahti, M., et al. (2022). Donor N-Substitution as Design Principle for Fast and Blue Luminescence in Carbene-Metal-Amides. Advanced Optical Materials https://doi.org/10.1002/adom.202200312
Description
Funder: Academy of Finland : Flagship Programme “Photonics Research and Innovation”; Grant(s): 320166
Funder: Osk. Huttunen Foundation; Id: http://dx.doi.org/10.13039/501100013507
Abstract
Abstract: A series of gold‐centered carbene‐metal‐amide (CMA) complexes are synthesized with the carbazole donor ligand modified by substitution with nitrogen atoms in varying positions. The luminescence of new aza‐CMA complexes shows a significant blueshift depending on the position of the N atom, to provide bright blue‐green (500 nm), sky‐blue (478 nm), blue (450 nm) and deep‐blue (419 nm) light‐emitters. The impact of the electron‐withdrawing aza‐group on the nature of the luminescence and the excited state energies of the locally excited (LE) or charge transfer (CT) states have been interpreted with the help of transient absorption, in‐depth photoluminescence experiments and theoretical calculations. By considering the orbital characters of the lowest CT and LE states, we develop a new concept for simultaneous energy tuning for both of these states with a single aza‐substitution, allowing for fast and blue CT emission. This concept allows the interference of 3LE phosphorescence to be avoided at room temperature. The approach is extended to two N substitutions at the optimal location in the 3‐ and 6‐positions of the carbazole skeleton. These results suggest a practical molecular design towards the development of bright and deep‐blue emitting CMA materials to tackle the stability problem of energy‐efficient deep‐blue OLEDs.
Keywords
Research Article, Research Articles, carbazole, carbene‐metal‐amide, gold, phosphorescence, thermally activated delayed fluorescence
Sponsorship
European Research Council (ERC) Advanced Investigator Award (338944‐GOCAT)
Royal Society (URF\R1\180288, RGF\EA\181008, RGF\EA\180041)
Finnish Grid and Cloud Infrastructure resources (2016072533)
Engineering and Physical Sciences Research Council (EP/K039547/1)
Identifiers
adom202200312
External DOI: https://doi.org/10.1002/adom.202200312
This record's URL: https://www.repository.cam.ac.uk/handle/1810/337345
Rights
Licence:
http://creativecommons.org/licenses/by/4.0/
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