Multivariate Analysis Identifying [Cu(N boolean AND N)(P boolean AND P)](+) Design and Device Architecture Enables First-Class Blue and White Light-Emitting Electrochemical Cells

ADVANCED MATERIALS(2022)

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摘要
White light-emitting electrochemical cells (LECs) comprising only [Cu(N<^>N)(P<^>P)](+) have not been reported yet, as all the attempts toward blue-emitting complexes failed. Multivariate analysis, based on prior-art [Cu(N<^>N)(P<^>P)](+)-based thin-film lighting (>90 papers) and refined with computational calculations, identifies the best blue-emitting [Cu(N<^>N)(P<^>P)](+) design for LECs, that is, N<^>N: 2-(4-(tert-butyl)phenyl)-6-(3,5-dimethyl-1H-pyrazol-1-yl)pyridine and P<^>P: 4,5-bis(diphenylphosphino)-9,9-dimethylxanthene, to achieve predicted thin-film emission at 490 nm and device performance of 3.8 cd A(-1)@170 cd m(-2). Validation comes from synthesis, X-ray structure, thin-film spectroscopic/microscopy/electrochemical characterization, and device optimization, realizing the first [Cu(N<^>N)(P<^>P)](+)-based blue-LEC with 3.6 cd A(-1)@180 cd m(-2). This represents a record performance compared to the state-of-the-art tricoordinate Cu(I)-complexes blue-LECs (0.17 cd A(-1)@20 cd m(-2)). Versatility is confirmed with the synthesis of the analogous complex with 2-(4-(tert-butyl)phenyl)-6-(3,5-dimethyl-1H-pyrazol-1-yl)pyrazine (N<^>N), showing a close prediction/experiment match: lambda = 590/580 nm; efficiency = 0.55/0.60 cd A(-1)@30 cd m(-2). Finally, experimental design is applied to fabricate the best white multicomponent host:guest LEC, reducing the number of trial-error attempts toward the first white all-[Cu(N<^>N)(P<^>P)](+)-LECs with 0.6 cd A(-1)@30 cd m(-2). This corresponds to approximately ten-fold enhancement compared to previous LECs (<0.05 cd A(-1)@<12 cd m(-2)). Hence, this work sets in the first multivariate approach to design emitters/active layers, accomplishing first-class [Cu(N<^>N)(P<^>P)](+)-based blue/white LECs that were previously elusive.
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关键词
blue emitters, copper(I) complexes, light-emitting electrochemical cells, multivariate design experiment, white lighting sources
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