Highly emissive excitons with reduced exchange energy in thermally activated delayed fluorescent molecules

A Pershin, D Hall, V Lemaur, JC Sancho-Garcia… - Nature …, 2019 - nature.com
Nature communications, 2019nature.com
Unlike conventional thermally activated delayed fluorescence chromophores, boron-
centered azatriangulene-like molecules combine a small excited-state singlet-triplet energy
gap with high oscillator strengths and minor reorganization energies. Here, using highly
correlated quantum-chemical calculations, we report this is driven by short-range
reorganization of the electron density taking place upon electronic excitation of these multi-
resonant structures. Based on this finding, we design a series of π-extended boron-and …
Abstract
Unlike conventional thermally activated delayed fluorescence chromophores, boron-centered azatriangulene-like molecules combine a small excited-state singlet-triplet energy gap with high oscillator strengths and minor reorganization energies. Here, using highly correlated quantum-chemical calculations, we report this is driven by short-range reorganization of the electron density taking place upon electronic excitation of these multi-resonant structures. Based on this finding, we design a series of π-extended boron- and nitrogen-doped nanographenes as promising candidates for efficient thermally activated delayed fluorescence emitters with concomitantly decreased singlet-triplet energy gaps, improved oscillator strengths and core rigidity compared to previously reported structures, permitting both emission color purity and tunability across the visible spectrum.
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