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

Published version
Peer-reviewed

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Authors

Credgington, Daniel  ORCID logo  https://orcid.org/0000-0003-4246-2118

Abstract

Carbene-metal-amides (CMAs) are a promising family of donor-bridge-acceptor molecular charge-transfer emitters for organic light-emitting diodes (OLEDs). Here a universal approach is introduced to tune the energy of their charge-transfer emission. A shift of up to 210 meV is achievable in the 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 the guest molecules and the polar host. This allows the emission of mid-green CMA archetypes to be blue shifted without chemical modifications. Monte-Carlo simulations based on a Marcus-type transfer integral successfully reproduce the concentration- and temperature-dependent triplet diffusion process, and reveal a substantial shift in the ensemble density of states in polar hosts. In gold-bridged CMAs this substantial shift does not lead to a significant change in luminescence lifetime, thermal activation energy, reorganisation energy or intersystem crossing rate. These discoveries thus offer new experimental and theoretical insight in to the coupling between the singlet and triplet manifolds in these materials. Similar emission tuning can be achieved in related materials where chemical modification is used to modify the charge-transfer energy.

Description

Keywords

carbene-metal-amide, coupling mechanism, emission tuning, organometallics, thermally-activated delayed fluorescence

Journal Title

Advanced Functional Materials

Conference Name

Journal ISSN

1616-301X
1616-3028

Volume Title

30

Publisher

Wiley-Blackwell
Sponsorship
Royal Society (RG140472)
Royal Society (RGF/EA/180041)
Engineering and Physical Sciences Research Council (EP/M005143/1)
Engineering and Physical Sciences Research Council (EP/L015978/1)