New design strategy for chemically-stable blue phosphorescent materials: improving the energy gap between theT1and3MC states

Abstract

A series of Ir- and Pt-based blue phosphorescent materials were theoretically investigated by means of density functional theory (DFT) calculations to improve their chemical stability in the excited state. High energy splitting between the lowest triplet state (T1state), generally a metal-to-ligand charge transfer state (3MLCT), and the triplet metal-centred state (3MC) can prohibit ligand dissociation and suppress the decomposition reaction from the3MC state to the dissociated S0. Here, we suggest a new design strategy to improve the chemical stability of blue phosphorescent materials in the excited state. Introducing inter- and intra-ligand interactions in Ir and Pt complexes can dramatically increase the ��E(3MC-T1) because attractive or repulsive couplings arising from intra- or inter-ligand interactions can effectively prevent the out-of-plane bending vibrational mode in Ir complexes and the ring deformation vibrational mode in Pt complexes. A ��E(3MC-T1) values of 18.62 kcal mol?1for an Ir complex and 22.86 kcal mol?1for a Pt complex from theT1energy were obtained while theT1energy was maintained in the blue region. To the best of our knowledge, these are the highest ��E(3MC-T1) values reported to date. We believe that the present research provides profound insights into the excited state chemical stability of deep blue phosphorescent materials that could be implemented to improve device lifetimes. ? the Owner Societies 2021.