Adding a twist for enhanced performance: The efficiency of organic light-emitting diodes (OLEDs) is fundamentally governed by the ratio of emissive singlet to dark triplet excitons that are formed from spin-polarized electron and hole currents within the material. Typically, this has set an upper limit of 25% internal quantum efficiency for OLEDs. Di et al. manipulated the ratio of spin states through a modification of process chemistry. They introduced a rotation of the molecular structure, which inverted the spin-state energetics and enhanced OLED performance. Science , this issue p. 159
Conformationally flexible “Carbene–Metal–Amide” (CMA) complexes of copper and gold have been developed based on a combination of sterically hindered cyclic (alkyl)(amino)carbene (CAAC) and 6- and 7-ring heterocyclic amide ligands. These complexes show photoemissions across the visible spectrum with PL quantum yields of up to 89% in solution and 83% in host-guest films. Single crystal X-ray diffraction and photoluminescence (PL) studies combined with DFT calculations indicate the important role of ring structure and conformational flexibility of the amide ligands. Time-resolved PL shows efficient delayed emission with sub-microsecond to microsecond excited state lifetimes at room temperature, with radiative rates exceeding 106 s−1. Yellow organic light-emitting diodes (OLEDs) based on a 7-ring gold amide were fabricated by thermal vapor deposition, while the sky-blue to warm-white mechanochromic behavior of the gold phenothiazine-5,5-dioxide complex enabled fabrication of the first CMA-based white light-emitting OLED.