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Article: Cu(I) and Ag(I) Complexes with a New Type of Rigid Tridentate N,P,P-Ligand for Thermally Activated Delayed Fluorescence and OLEDs with High External Quantum Efficiency
Title | Cu(I) and Ag(I) Complexes with a New Type of Rigid Tridentate N,P,P-Ligand for Thermally Activated Delayed Fluorescence and OLEDs with High External Quantum Efficiency |
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Authors | |
Issue Date | 2020 |
Publisher | American Chemical Society. The Journal's web site is located at http://pubs.acs.org/cm |
Citation | Chemistry of Materials, 2020, v. 32 n. 24, p. 10365-10382 How to Cite? |
Abstract | Neutral Cu(I) and Ag(I) complexes with a new rigid tridentate N,P,P ligand (dmpzpp, 3,5-dimethyl-1-(2-((2-(di-o-tolyl)phosphanyl) (o-tolyl)-phosphanyl)phenyl)-1H-pyrazole), giving Cu(dmpzpp)Cl 6, Cu(dmpzpp)Br 7, Cu(dmpzpp)I 8, Cu(dmpzpp)SPh 9, and Ag(dmpzpp)I 10 with SPh = thiophenylato, were prepared and their crystal structures, TD-DFT electronic structures, and phosphorescence and thermally activated delayed fluorescence (TADF) properties were studied in detail. The photoluminescence quantum yields ΦPL of neat powder materials lie between 70 and 90% with emission colors from blue to yellow. Compound 9, with bulky ligands showing ΦPL = 90%, was used for detailed emission studies from T = 1.7 to 300 K. Up to T ≈ 70 K, 9 shows only long-lived phosphorescence with a radiative decay time of T1 of τr(phos) = 1 ms because of weak spin–orbit coupling. Accordingly, the zero-field splittings of T1 in three substates are < 1 cm–1 (0.1 meV). Individual decay times of 2400, 2250, and 292 μs are estimated. Presumably, the phosphorescence is essentially induced by spin–vibronic mechanisms. Up to T = 300 K, the radiative decay time decreases by more than two orders of magnitude to τr(TADF) = 5.6 μs because of the TADF effect. This short decay time is determined by the small gap of ΔE(S1–T1) = 600 cm–1 (74 meV) and the fast radiative S1 → S0 rate of 1.1 × 107 s–1 (91 ns). For fabrication of OLED devices, we applied sublimable 8 and 9 using cohost device structures. For example, with a concentration of 2 wt % of 8, a green-emitting OLED showing CIE coordinates of (0.33; 0.52), a high external quantum efficiency of up to EQE = 16.4%, and a high luminance of almost 10,000 cd m–2 could be fabricated. Strategies for designing compounds giving higher EQE are presented. |
Persistent Identifier | http://hdl.handle.net/10722/302374 |
ISSN | 2023 Impact Factor: 7.2 2023 SCImago Journal Rankings: 2.421 |
ISI Accession Number ID |
DC Field | Value | Language |
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dc.contributor.author | Klein, M | - |
dc.contributor.author | Rau, N | - |
dc.contributor.author | Wende, M | - |
dc.contributor.author | Sundermeyer, J | - |
dc.contributor.author | Cheng, G | - |
dc.contributor.author | Che, CM | - |
dc.contributor.author | Schinabeck, A | - |
dc.contributor.author | Yersin, H | - |
dc.date.accessioned | 2021-09-06T03:31:22Z | - |
dc.date.available | 2021-09-06T03:31:22Z | - |
dc.date.issued | 2020 | - |
dc.identifier.citation | Chemistry of Materials, 2020, v. 32 n. 24, p. 10365-10382 | - |
dc.identifier.issn | 0897-4756 | - |
dc.identifier.uri | http://hdl.handle.net/10722/302374 | - |
dc.description.abstract | Neutral Cu(I) and Ag(I) complexes with a new rigid tridentate N,P,P ligand (dmpzpp, 3,5-dimethyl-1-(2-((2-(di-o-tolyl)phosphanyl) (o-tolyl)-phosphanyl)phenyl)-1H-pyrazole), giving Cu(dmpzpp)Cl 6, Cu(dmpzpp)Br 7, Cu(dmpzpp)I 8, Cu(dmpzpp)SPh 9, and Ag(dmpzpp)I 10 with SPh = thiophenylato, were prepared and their crystal structures, TD-DFT electronic structures, and phosphorescence and thermally activated delayed fluorescence (TADF) properties were studied in detail. The photoluminescence quantum yields ΦPL of neat powder materials lie between 70 and 90% with emission colors from blue to yellow. Compound 9, with bulky ligands showing ΦPL = 90%, was used for detailed emission studies from T = 1.7 to 300 K. Up to T ≈ 70 K, 9 shows only long-lived phosphorescence with a radiative decay time of T1 of τr(phos) = 1 ms because of weak spin–orbit coupling. Accordingly, the zero-field splittings of T1 in three substates are < 1 cm–1 (0.1 meV). Individual decay times of 2400, 2250, and 292 μs are estimated. Presumably, the phosphorescence is essentially induced by spin–vibronic mechanisms. Up to T = 300 K, the radiative decay time decreases by more than two orders of magnitude to τr(TADF) = 5.6 μs because of the TADF effect. This short decay time is determined by the small gap of ΔE(S1–T1) = 600 cm–1 (74 meV) and the fast radiative S1 → S0 rate of 1.1 × 107 s–1 (91 ns). For fabrication of OLED devices, we applied sublimable 8 and 9 using cohost device structures. For example, with a concentration of 2 wt % of 8, a green-emitting OLED showing CIE coordinates of (0.33; 0.52), a high external quantum efficiency of up to EQE = 16.4%, and a high luminance of almost 10,000 cd m–2 could be fabricated. Strategies for designing compounds giving higher EQE are presented. | - |
dc.language | eng | - |
dc.publisher | American Chemical Society. The Journal's web site is located at http://pubs.acs.org/cm | - |
dc.relation.ispartof | Chemistry of Materials | - |
dc.rights | This document is the Accepted Manuscript version of a Published Work that appeared in final form in Chemistry of Materials, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/acs.chemmater.0c02683 | - |
dc.title | Cu(I) and Ag(I) Complexes with a New Type of Rigid Tridentate N,P,P-Ligand for Thermally Activated Delayed Fluorescence and OLEDs with High External Quantum Efficiency | - |
dc.type | Article | - |
dc.identifier.email | Che, CM: chemhead@hku.hk | - |
dc.identifier.authority | Cheng, G=rp02145 | - |
dc.identifier.authority | Che, CM=rp00670 | - |
dc.description.nature | postprint | - |
dc.identifier.doi | 10.1021/acs.chemmater.0c02683 | - |
dc.identifier.scopus | eid_2-s2.0-85097749737 | - |
dc.identifier.hkuros | 324867 | - |
dc.identifier.volume | 32 | - |
dc.identifier.issue | 24 | - |
dc.identifier.spage | 10365 | - |
dc.identifier.epage | 10382 | - |
dc.identifier.isi | WOS:000603288800007 | - |
dc.publisher.place | United States | - |