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Carbene-metal-amides (CMAs) are a promising family of donor-bridge-acceptormolecular charge-transfer emitters for organic light-emitting diodes (OLEDs).Here a universal approach is introduced to tune the energy of theircharge-transfer emission. A shift of up to 210 meV is achievable in the solidstate via dilution in a polar host matrix. The origin of this shift has twocomponents: constraint of thermally activated triplet diffusion, andelectrostatic interactions between the guest molecules and the polar host. Thisallows the emission of mid-green CMA archetypes to be blue shifted withoutchemical modifications. Monte-Carlo simulations based on a Marcus-type transferintegral successfully reproduce the concentration- and temperature-dependenttriplet diffusion process, and reveal a substantial shift in the ensembledensity of states in polar hosts. In gold-bridged CMAs this substantial shiftdoes not lead to a significant change in luminescence lifetime, thermalactivation energy, reorganisation energy or intersystem crossing rate. Thesediscoveries thus offer new experimental and theoretical insight in to thecoupling between the singlet and triplet manifolds in these materials. Similaremission tuning can be achieved in related materials where chemicalmodification is used to modify the charge-transfer energy.

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