Abstract:We demonstrate a new approach to utilize copper(I) iodide coordination complexes as emissive layers in organic light-emitting diodes (OLEDs), by in situ codeposition of copper(I) iodide and 3,5-bis(carbazol-9-yl)pyridine (mCPy). With a simple three-layer device structure, pure green electroluminescence at 530 nm from a copper(I) complex was observed. Maximum luminance and external quantum efficiency (EQE) of 9700 cd/m2 and 4.4% have been achieved, respectively. The luminescent species has been identified as [C… Show more
“…[1][2][3][4][5][6][7][8] The interest stems from the increasing demand of more-affordable complexes in preference to luminescent metal complexes based on precious (i.e. the platinum group) and rare-earth metals, which are oen quite expensive and environmentally problematic.…”
The copper iodide complexes are known for their large variety of coordination geometries. Such diversity, while making it difficult to predict the final structure, permits the preparation of a great number of copper iodide complexes based on the same ligand. The target of the research was that of thoroughly exploring the chemistry of CuI and the ligand diphenyl-2-pyridyl phosphine (PN) by varying the stoichiometric ratio and/or the aggregation state. Six different compounds have been identified: [Cu4I4(PN)2], [Cu4I4(PN)2·(CH2Cl2)0.5], [CuI(PN)0.5]∞, [CuI(PN)3] whose structures have been determined during this study, CuI(PN)2 which was characterized by powder diffraction and [Cu2I2(PN)3] which has been already reported. The preparation routes are also different: synthesis in solution yielded [Cu4I4(PN)2·(CH2Cl2)0.5] and [CuI(PN)3] while [CuI(PN)0.5]∞ and CuI(PN)2 were obtained only via solid state reactions. These two latter examples confirmed that mechanochemistry is a valid route to explore the landscape of the possible structures of CuI derivatives. Crystallization by traditional solution procedures failed to give the desired crystal, so structure determination of the new compounds was tackled in two ways: by attempting crystal growth via solvothermal synthesis and by resolving the structure from X-ray powder diffraction data with "direct space" methods. What is more the photophysical properties of the complexes that could be obtained as sufficiently pure powders have also been investigated and are reported herein.
“…[1][2][3][4][5][6][7][8] The interest stems from the increasing demand of more-affordable complexes in preference to luminescent metal complexes based on precious (i.e. the platinum group) and rare-earth metals, which are oen quite expensive and environmentally problematic.…”
The copper iodide complexes are known for their large variety of coordination geometries. Such diversity, while making it difficult to predict the final structure, permits the preparation of a great number of copper iodide complexes based on the same ligand. The target of the research was that of thoroughly exploring the chemistry of CuI and the ligand diphenyl-2-pyridyl phosphine (PN) by varying the stoichiometric ratio and/or the aggregation state. Six different compounds have been identified: [Cu4I4(PN)2], [Cu4I4(PN)2·(CH2Cl2)0.5], [CuI(PN)0.5]∞, [CuI(PN)3] whose structures have been determined during this study, CuI(PN)2 which was characterized by powder diffraction and [Cu2I2(PN)3] which has been already reported. The preparation routes are also different: synthesis in solution yielded [Cu4I4(PN)2·(CH2Cl2)0.5] and [CuI(PN)3] while [CuI(PN)0.5]∞ and CuI(PN)2 were obtained only via solid state reactions. These two latter examples confirmed that mechanochemistry is a valid route to explore the landscape of the possible structures of CuI derivatives. Crystallization by traditional solution procedures failed to give the desired crystal, so structure determination of the new compounds was tackled in two ways: by attempting crystal growth via solvothermal synthesis and by resolving the structure from X-ray powder diffraction data with "direct space" methods. What is more the photophysical properties of the complexes that could be obtained as sufficiently pure powders have also been investigated and are reported herein.
“…[1][2][3][4][5][6][7][8][9][10][11] This class of compounds is attracting renewed interest 12-16 because of its potential applications in highefficiency OLEDs. [17][18][19] Coordination systems based on copper halides show a remarkable structural diversity, 15 which arises from the many possible combinations of coordination numbers (two, three and four) available for copper(I) and for the geometries that can be adopted by the halide ions (from terminal to m 2 -and up to m 8 -bridging modes).…”
Reactions between copper(I) iodide and triphenylphosphine have been explored in solution and in the solid state and six luminescent coordination complexes have been obtained and characterized by X-ray diffraction and UV-vis spectroscopy and photophysics. Solid-state reactions of CuI with PPh(3) in different conditions (kneading, vapour digestion) and stoichiometries resulted in the formation of high ratio ligand:metal compounds while tetrameric structures could be obtained only by solution reactions. Crystal structures were determined by single crystal X-ray diffraction while purity of the bulk product was checked by powder diffraction (XRPD). Three different tetrameric structures with 1:1 stoichiometry have been synthesized: two closed cubane-type polymorphs [CuI(PPh(3))](4) (form 1a) and [CuI(PPh(3))](4) (form 1b) and an open step-like isomer [CuI(PPh(3))](4) (form 2). The conversions between the polymorphs and isomers have been studied and characterized by XRPD. The most stable form [CuI(PPh(3))](4) (form 1b) can convert into the open step-like isomer [CuI(PPh(3))](4) (form 2) in a slurry experiment with EtOH or CH(2)Cl(2) or AcCN and converts back into [CuI(PPh(3))](4)1b when exposed to vapors of toluene. At room temperature all the tetrameric compounds exhibit luminescence in the solid state and, notably, the two polymorphs show a dissimilar dual emission at low temperature. The luminescence features in the solid state seem to be peculiarly related to the presence of the aromatic phosphine ligand and depend on the Cu-Cu distance in the cluster.
“…in 2011[101] using 3,5-bis(carbazol-9-yl)pyridine (mCPy) as ligand. With a simple three-layer device structure, pure green electroluminescence at 530 nm with maximum EQE of 4.4 % and luminance of 9700 cd/m 2 was reported for the complex [CuI(mCPy) 2 ] 2 , 106 (Figure 24).…”
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