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| Naji, M. |
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| Motta, Antonella |
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| Aletan, Dirar |
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| Mohamed, Tarek |
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| Ertürk, Emre |
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| Taccardi, Nicola |
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| Kononenko, Denys |
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| Petrov, R. H. | Madrid |
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| Alshaaer, Mazen | Brussels |
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| Bih, L. |
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| Casati, R. |
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| Muller, Hermance |
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| Kočí, Jan | Prague |
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| Šuljagić, Marija |
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| Kalteremidou, Kalliopi-Artemi | Brussels |
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| Azam, Siraj |
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| Ospanova, Alyiya |
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| Blanpain, Bart |
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| Ali, M. A. |
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| Popa, V. |
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| Rančić, M. |
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| Ollier, Nadège |
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| Azevedo, Nuno Monteiro |
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| Landes, Michael |
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| Rignanese, Gian-Marco |
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Zysman-Colman, Eli
University of St Andrews
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (21/21 displayed)
- 2024Organic light-emitting diodes comprising an undoped thermally activated delayed fluorescence emissive layer and a thick inorganic perovskite hole transport layer
- 2024Organic Light-Emitting Diodes Comprising an Undoped Thermally Activated Delayed Fluorescence Emissive Layer and a Thick Inorganic Perovskite Hole Transport Layer
- 2021A luminescent 1D silver polymer containing [2.2]paracyclophane ligandscitations
- 2020A Pd 3 L 6 supramolecular cage incorporating photoactive [2.2]paracyclophane unitscitations
- 2020Stable 6H organic-inorganic hybrid lead perovskite and competitive formation of 6H and 3C perovskite structure with mixed A cationscitations
- 2020A Pd3L6 supramolecular cage incorporating photoactive [2.2]paracyclophane Unitscitations
- 2020What controls the orientation of TADF emitters?citations
- 2019A Pd 3 L 6 supramolecular cage incorporating photoactive [2.2]paracyclophane Unitscitations
- 2019Stable 6H organic-inorganic hybrid lead perovskite and competitive formation of 6H and 3C perovskite structure with mixed A cationscitations
- 2019A Pd3L6 supramolecular cage incorporating photoactive [2.2]paracyclophane Unitscitations
- 2017Lessons learned in tuning the optoelectronic properties of phosphorescent iridium(III) complexescitations
- 2017Blue-to-green emitting neutral Ir(III) complexes bearing pentafluorosulfanyl groups:a combined experimental and theoretical studycitations
- 2017Blue-to-green emitting neutral Ir(III) complexes bearing pentafluorosulfanyl groups : a combined experimental and theoretical studycitations
- 2017Blue-to-green emitting neutral Ir(III) complexes bearing pentafluorosulfanyl groupscitations
- 2016Synthesis and characterization of green-to-yellow emissive Ir(III) complexes of pyridylbenzothiadiazine ligandcitations
- 2016Enhancing the photoluminescence quantum yields of blue-emitting cationic iridium(III) complexes bearing bisphosphine ligandscitations
- 2016Enhancing the photoluminescence quantum yields of blue-emitting cationic iridium(III) complexes bearing bisphosphine ligandscitations
- 2016Synthesis, properties and Light-Emitting Electrochemical Cell (LEEC) device fabrication of cationic Ir(III) complexes bearing electron-withdrawing groups on the cyclometallating ligandscitations
- 2016Synthesis, properties and Light-Emitting Electrochemical Cell (LEEC) device fabrication of cationic Ir(III) complexes bearing electron-withdrawing groups on the cyclometallating ligandscitations
- 2015Strategic modulation of the photonic properties of conjugated organometallic Pt–Ir polymers exhibiting hybrid CT-excited statescitations
- 2014Strategic modulation of the photonic properties of conjugated organometallic Pt–Ir polymers exhibiting hybrid CT-excited statescitations
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article
Blue-to-green emitting neutral Ir(III) complexes bearing pentafluorosulfanyl groups
Abstract
A structure-property relationship study of neutral heteroleptic (<b>1</b> and <b>2</b>, [Ir(C^N)<sub>2</sub>(L^X)]) and homoleptic (<b>3</b> and <b>4</b>, <i>fac</i>-[Ir(C^N)<sub>3</sub>]) Ir(III) complexes [where L^X = anionic 2,2,6,6-tetramethylheptane-3,5-dionato-<i>κO</i><sup>3</sup>,<i>κO</i><sup>6</sup> (thd) and C^N = a cyclometalating ligand bearing a pentafluorosulfanyl (-SF<sub>5</sub>) electron-withdrawing group (EWG) at C4 (H<b>L1</b>) and C3 (H<b>L2</b>) positions of the phenyl moiety] is presented. These complexes have been fully structurally characterised, including by single crystal X-ray diffraction, and their electrochemical and optical properties have also been extensively studied. While complexes <b>1</b> ([Ir(<b>L1</b>)2(thd)]), <b>3</b> (Ir(<b>L1</b>)3) and <b>4</b> (Ir(<b>L2</b>)3) exhibit irreversible first reduction waves based on the pentafluorosulfanyl substituent in the range of -1.71 V to -1.88 V (<i>vs</i>. SCE), complex <b>2</b> ([Ir(<b>L2</b>)2(thd)]) exhibits a quasi-reversible pyridine<sub>C^N</sub>-based first reduction wave that is anodically-shifted at -1.38 V. The metal+C^N ligand oxidation waves are all quasi-reversible in the range of 1.08-1.54 V (<i>vs</i>. SCE). The optical gap, determined from the lowest energy absorption maxima, decreases from <b>4</b> to <b>2</b> to <b>3</b> to <b>1</b> and this trend is consistent with the Hammett behaviour (σ<sub>m</sub>/σ<sub>p</sub> with respect to the metal-carbon bond) of the –SF<sub>5</sub> EWG. In degassed acetonitrile, for complexes <b>2</b>-<b>4</b>, introduction of the -SF<sub>5</sub> group produced a blue-shifted emission (λ<sub>em</sub> = 484-506 nm) compared to reference complexes [Ir(ppy)<sub>2</sub>(acac)], <b>R1</b> (where acac = acetylacetonato) (λ<sub>em</sub> = 528 nm in MeCN), [Ir(CF<sub>3</sub>-ppy)(acac)], <b>R3</b> (where CF<sub>3</sub>-ppy = 2-(4-(trifluoromethyl)phenyl)pyridine) (λ<sub>em</sub> = 522 nm in DCM) and [Ir(CF<sub>3</sub>-ppy)<sub>3</sub>], <b>R8</b> (λem = 507 nm in MeCN). The emission of complex <b>1</b>, by contrast, was modestly red-shifted (λem = 534 nm). Complexes <b>2</b> and <b>4</b>, where the –SF<sub>5</sub> EWG is substituted para to the Ir-C<sub>ppy</sub> bond are efficient phosphorescent emitters, with high photoluminescence quantum yields (Φ<sub>PL</sub> = 58-79% in degassed MeCN solution) and microsecond emission lifetimes (τ<sub>ε</sub> = 1.35-3.02 μs). Theoretical and experimental observations point towards excited states that are principally ligand-centered (<sup>3</sup>LC) in nature, but with a minor metal-to-ligand charge-transfer (<sup>3</sup>MLCT) transition component, as a function of the regiochemistry of the pentafluorosulfanyl group. The <sup>3</sup>LC character is predominant over the mixed <sup>3</sup>CT character for complexes <b>1</b>, <b>2</b> and <b>4</b> while in complex <b>3</b>, there is exclusive <sup>3</sup>LC character as demonstrated by unrestricted Density Functional Theory (DFT) calculations. The short emission lifetimes and reasonable Φ<sub>PL</sub> values in doped thin film (5 wt% in PMMA), particularly for <b>4</b>, suggest that these neutral complexes would be attractive candidate emitters in organic light-emitting diodes.