transition metal complexes as phosphorescent emitters, making it possible to harvest both singlet and triplet excitons leading to 100% electroluminescence quantum efficiency. [2] Cyclometalated iridium(III) complexes have emerged as one of the most promising triplet emitters because of their versatile color tunability, chemical stability, good thermal properties, and high photoluminescent quantum yields (Φ PL ). [3][4][5][6][7] These phosphors often involve an octahedral Ir 3+ ion with bidentate ligands, C^N:, comprised of a covalently bonded aryl moiety and a datively bonded nitrogen group, such as pyridyl, to give a tris-cyclometalated complex, Ir(C^N:) 3 . While efficient OLEDs using red and green Ir-based phosphorescent emitters are commercially viable, [8][9][10] the stability of OLEDs using blue-emitting transition metal containing complexes are presently insufficient for practical applications. [11] Recently cyclometalated N-heterocyclic carbene (NHC)-Ir based chromophores, Ir(C^C:) 3 , have attracted attention due to their promising properties as blue emitters. [12][13][14][15][16][17][18][19] These C^C: based emitters have an aryl group as do C^N: ligands, but utilize a carbene in place of the nitrogen basic moiety. Our group reported one of the first blue-emitting Ir-carbene complexes for OLEDs, using N-phenyl, N-methyl-imidazol-2-yl (pmi) and N-phenyl, N-methyl-benzimidazol-2-yl (pmb) ligands. [16] Since then, several homoleptic [20][21][22][23] and heteroleptic [18] derivatives of these complexes have also been reported. These Ir(C^C:) 3 complexes have advantages over blue emissive Ir(C^N:) 3 complexes as they do not suffer from deactivation of the excited state via thermal population of triplet metal-centered ( 3 MC) states, which can severely diminish their Φ PL . Replacing the nitrogen basic moiety in the C^N: ligand with a strong field carbene ligand, largely mitigates this problem by destabilizing the 3 MC states, which makes them thermally inaccessible. Interestingly, it was found that even when the 3 MC states are thermally populated, the carbene iridium complexes were able to undergo reversible population of the radiative state leaving the Ir-carbene bond intact. [24] Since the Ir-N bond dissociation in the excited state has been shown to be problematic in Ir(C^N:) 3 complexes, [4] computational results have suggested that replacement with the stronger IrC carbene bond will result in a more robust emitter. [24,25] Further work on Ir(C^C:) 3 complexes led to the use of the electrophilic N-phenyl, N-methyl-pyridylimidazol-2-yl ligand The photophysical and electrochemical properties of N-heterocyclic carbene complexes of Iridium (III) (Ir(C^C:) 3 , where C^C: = N-phenyl,N-methylpyrazinoimidazol-2-yl (pmpz), N,N-di-p-tolyl-pyrazinoimidazol-2-yl (tpz)) are reported. Facial and meridional isomers of Ir(pmpz) 3 are prepared, but only the facial isomer can be isolated for Ir(tpz) 3 . The fac-Ir(pmpz) 3 and fac-Ir(tpz) 3 complexes have emission maxima at 465 nm in polystyrene, whereas the emission max...