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Environmental Control of Triplet Emission in Donor–Bridge–Acceptor Organometallics

Feng, J; Yang, L; Romanov, AS; Ratanapreechachai, J; Reponen, AM; Jones, STE; Linnolahti, M; ... Credgington, D; + view all (2020) Environmental Control of Triplet Emission in Donor–Bridge–Acceptor Organometallics. Advanced Functional Materials , 30 (9) , Article 1908715. 10.1002/adfm.201908715. Green open access

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Abstract

Carbene-metal-amides (CMAs) are a promising family of donor–bridge–acceptor molecular charge-transfer (CT) emitters for organic light-emitting diodes. A universal approach is demonstrated to tune the energy of their CT emission. A blueshift of up to 210 meV is achievable in solid state via dilution in a polar host matrix. The origin of this shift has two components: constraint of thermally-activated triplet diffusion, and electrostatic interactions between guest and polar host. This allows the emission of mid-green CMA archetypes to be tuned to sky blue without chemical modifications. Monte-Carlo simulations based on a Marcus-type transfer integral successfully reproduce the concentration- and temperature-dependent triplet diffusion process, revealing a substantial shift in the ensemble density of states in polar hosts. In gold-bridged CMAs, this shift does not lead to a significant change in luminescence lifetime, thermal activation energy, reorganization energy, or intersystem crossing rate. These discoveries offer new insight into coupling between the singlet and triplet manifolds in CMA materials, revealing a dominant interaction between states of CT character. The same approach is employed using materials which have been chemically modified to alter the energy of their CT state directly, shifting the emission of sky-blue chromophores into the practical blue range.

Type: Article
Title: Environmental Control of Triplet Emission in Donor–Bridge–Acceptor Organometallics
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/adfm.201908715
Publisher version: https://doi.org/10.1002/adfm.201908715
Language: English
Additional information: This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10136205
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