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Solvent-Dependent Sensitization of Ytterbium and Neodymium via an Intramolecular Excimer
摘要： We report the synthesis of a di(1-pyrenyl)-phosphoryl acetophenone ligand containing two pyrenyl moieties linked by a single phosphorus atom. The ligand exhibits solvent-dependent emission: in nonpolar solvents, typical monomeric pyrene emission is observed, whereas in polar solvents, an additional broad and structureless emission appears. The emission in polar solvents is concentration independent and is attributed to the emission of an intramolecular excimer. The coordination of the di(1-pyrenyl)phosphoryl acetophenone ligand as well as the corresponding deprotonated anionic di(1-pyrenyl)phosphoryl acetophenonate ligand was studied with the near-infrared emitting lanthanides, neodymium and ytterbium. Solvent-dependent sensitization of both lanthanides was observed and correlates with the presence of the excimer emission. Sensitization of ytterbium is more efficient than neodymium, and the overall quantum yields were found to be 12.8 and 1.9% for ytterbium and neodymium, respectively.
关键词： solvent-dependent emission,quantum yields,ytterbium,neodymium,intramolecular excimer,lanthanides
更新于2025-11-14 15:24:45
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Solar photodegradation of oxytetracycline in brackish aquaculture water: New insights about effects of Ca2+ and Mg2+
摘要： Oxytetracycline (OTC) is an antibiotic used in aquaculture able to complex with the major cations Ca2+ and Mg2+, existing in brackish water. The effects of these cations on the solar photodegradation of OTC have been investigated. Calcium promotes a faster OTC photo-degradation in aqueous solution, while the same does not occur with Mg2+. For some authors the accelerating effect of Ca2+ is attributed to the occurrence of self-sensitized photodegradation of the complexes with Ca2+, which is not possible in the complexes with Mg2+, due to different binding patterns of these cations. In this work, the controversy concerning the binding sites of these cations in OTC is discussed. Based on spectroscopic evidence, similar binding patterns of OTC with Ca2+ and Mg2+ and a lower quantum yield of the direct photolysis of the complexes with Mg2+ are proposed. In addition, it was demonstrated that Mg2+ inhibits the formation of some OTC photoproducts observed in the presence of Ca2+, while at least two new OTC photoproducts are formed in the presence of Mg2+.
关键词： Photoproducts,Complexes,Quantum yields,Antibiotic,Photolysis,Spectroscopy
更新于2025-09-23 15:22:29
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Aggregation-induced Emission Polymers for High Performance PLEDs with Low Efficiency Roll-off
摘要： As the congener of organic light-emitting diodes, polymeric light-emitting diodes (PLEDs) possess a number of distinct merits such as low-cost wet fabrication process, which enable them applicable in large-area flexible display and lighting fields. However, most emissive polymers used in PLEDs suffer from the aggregation-caused quenching (ACQ) effect, which makes the device show large efficiency roll-off. In this work, two polymers of pTPE-TPA-Cz and pTPE-TPA-Flu featuring aggregation-induced emission (AIE) characteristics were facilely synthesized through Suzuki-Miyaura polycoupling reaction by incorporating the AIE unit of TPE-TPA in their main chains. The resultant polymers possess good film-forming ability, excellent thermal stability and high photoluminescence quantum yields (PLQY) in their film states, facilitating the fabrication of PLEDs through solution process. Indeed, the PLEDs using pTPE-TPA-Cz and pTPE-TPA-Flu as emitting layers (EMLs) could achieve a maximum external quantum efficiency (EQE) of 3.26% (doped EML) and current efficiency of 3.69 cd A-1 (non-doped EML). Notably, all the devices exhibit a quite low efficiency roll-off. This work indicates that AIE polymers are ideal candidates for the construction high performance PLEDs with low efficiency roll-off.
关键词： Aggregation-induced emission,Photoluminescence quantum yields,Solution process,Efficiency roll-off,Polymeric light-emitting diodes
更新于2025-09-23 15:21:01
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Mn-doped 2D Sn-based perovskites with energy transfer from self-trapped excitons to dopants for warm white light-emitting diodes
摘要： Mn-doped 2D perovskite powders are promising phosphors for warm white light-emitting diodes (LEDs). However, it remains a challenge to solve the problem of lead toxicity and improve photoluminescence quantum yields (PLQYs). Here, we have successfully prepared Mn-doped 2D Sn-based perovskite materials ((C8H17NH2)2Sn1-xMnxBr4). The PLQYs of (C8H17NH2)2Sn1-xMnxBr4 (x = 0.26) powders reach up to 42%. The as-prepared (C8H17NH2)2Sn1-xMnxBr4 exhibit a single broad photoluminescence (PL) band, differing from the dual peaks of Mn-doped lead halide perovskite quantum dots. Theoretical conclusions and experimental results show the competitive relationship between self-trapped excitons (STEs) emission from the host crystal and dopant Mn d-d transition emission. With Mn dopant concentration increasing, the PL spectra exhibit red shifts and the full width at half-maximum (FWHM) turns larger, which is constructive for warm white LEDs. The fabricated warm white LEDs based on (C8H17NH2)2Sn1-xMnxBr4 show warm white light correlated color temperature (CCT, 3542 K) and high color-rendering index (Ra, 88.12). Our work provides new possibilities for optoelectronic devices based on lead-free perovskite materials.
关键词： self-trapped excitons,Mn-doped,photoluminescence quantum yields,2D Sn-based perovskites,warm white light-emitting diodes
更新于2025-09-23 15:21:01
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Homoleptic mer-Ir(III) complexes for highly efficient solution-processable green phosphorescent organic light-emitting diodes with high current efficiency
摘要： Two new highly efficient homoleptic green-emitting meridional iridium (III) complexes namely, mer-tris[5-hexyl-8-trifluoromethyl-5H-benzo(c)(1,5)naphthyridin-6-one]iridium(III) (mer-Ir1) and mer-tris[5-ethylhexyl-8-trifluoromethyl-5H-benzo(c)(1,5)naphthyridin-6-one]iridium(III) (mer-Ir2) were designed and synthesized at high temperature. These new Ir(III) complexes consist of amide bridged trifluoromethyl substituted phenylpyridine skeleton with longer alkyl chain. Interestingly, both Ir(III) complexes, mer-Ir1 and mer-Ir2 show bright green emission (λmax = 528 nm) with high photoluminescence quantum yields of 42 and 51% in solution at room temperature, respectively. Their thermal, photophysical, electrochemical, and electroluminescent (EL) properties were fully investigated. Both complexes were used as dopants for solution-processed green phosphorescence organic light-emitting diodes (PHOLEDs). Notably, the device using mer-Ir2 as new green dopant exhibited excellent EL performance with a maximum external quantum efficiency of 20.03% and maximum current efficiency of 67.81 cd A-1. To the best of our knowledge, this is the first time, particularly Ir(C^N)3 based mer-Ir(III) isomers showing excellent EL performance with high luminous efficiency in the green region via solution-processed PHOLEDs has been reported.
关键词： high photoluminescence quantum yields,current efficiency,external quantum efficiency,homoleptic green-emitting meridional iridium (III) complexes,solution-processed green phosphorescence organic light-emitting diodes (PHOLEDs)
更新于2025-09-23 15:19:57
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Photophysical Impact of Diacetylenic Conjugation on Classical Donor-Acceptor Electronic Energy Pair
摘要： Organic fluorophores with extended π-conjugation are important for their wide-spread applications. The present work provides photophysical insights of a diacetylene bridged classical donor-acceptor electronic energy pair, naphthalene-pyrene, in comparison with its part molecular structures, naphthyl and pyrenyl acetylenes as well as parent naphthalene and pyrene chromophores. The diacetylenic dye loses individual spectral identities of the donor and acceptor fluorophores exhibiting a locally excited (LE) emission (~411 nm) from the overall molecular entity with high fluorescence quantum yields (0.55–0.84) in non-aqueous media. In contrast to parent pyrene, the hybrid derivative shows strongly allowed S0→S1 transition. In mixed-aqueous media, the dye forms J-aggregates displaying a new red-shifted absorption (~425 nm) as well as emission (~510 nm) band. Unlike the hybrid dye, the naphthyl and pyrenyl acetylenes do not form aggregates. In the aggregate state of the hybrid fluorophore, electronic energy transfer takes place from the naphthyl moiety to pyrenyl ring. The excited state photophysical properties of the dye is exploited to vapor sensing in solid state.
关键词： vapor sensing,Organic fluorophores,donor-acceptor electronic energy pair,diacetylene bridged,naphthalene-pyrene,locally excited emission,J-aggregates,electronic energy transfer,π-conjugation,fluorescence quantum yields
更新于2025-09-23 15:19:57
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Phosphane tuning in heteroleptic [Cu(N^N)(P^P)] <sup>+</sup> complexes for light-emitting electrochemical cells
摘要： The synthesis and characterization of five [Cu(P^P)(N^N)][PF6] complexes in which P^P = 2,7-bis(tert-butyl)-4,5-bis(diphenylphosphino)-9,9-dimethylxanthene (tBu2xantphos) or the chiral 4,5-bis(mesitylphenylphosphino)-9,9-dimethylxanthene (xantphosMes2) and N^N = 2,2’-bipyridine (bpy), 6-methyl-2,2’-bipyridine (6-Mebpy) or 6,6’-dimethyl-2,2’-bipyridine (6,6’-Me2bpy) are reported. Single crystal structures of four of the compounds confirm that the copper(I) centre is in a distorted tetrahedral environment. In [Cu(xantphosMes2)(6-Mebpy)][PF6], the 6-Mebpy unit is disordered over two equally populated orientations and this disorder parallels a combination of two dynamic processes which we propose for [Cu(xantphosMes2)(N^N)]+ cations in solution. Density functional theory (DFT) calculations reveal that the energy difference between the two conformers observed in the solid-state structure of [Cu(xantphosMes2)(6-Mebpy)][PF6] differ in energy by only 0.28 kcal mol?1. Upon excitation into the MLCT region (λexc = 365 nm), the [Cu(P^P)(N^N)][PF6] compounds are yellow to orange emitters. Increasing the number of Me groups in the bpy unit shifts the emission to higher energies, and moves the Cu+/Cu2+ oxidation to higher potentials. Photoluminescence quantum yields (PLQYs) of the compounds are low in solution, but in the solid state PLQYs of up to 59% (for [Cu(tBu2xantphos)(6,6’-Me2bpy)]+) are observed. Increased excited-state lifetimes at low temperature are consistent with the complexes exhibiting thermally activated delayed fluorescence (TADF). This is supported by the small energy difference calculated between the lowest-energy singlet and triplet excited states (0.17–0.25 eV). The compounds were tested in simple bilayer light-emitting electrochemical cells (LECs). The optoelectronic performances of complexes containing xantphosMes2 were generally lower with respect to those with tBu2xantphos, which led to bright and efficient devices. The best performing LECs were obtained for the complex [Cu(tBu2xantphos)(6,6’-Me2bpy)][PF6] due to the increased steric hindrance at the N^N ligand, resulting in higher PLQY.
关键词： photoluminescence quantum yields,heteroleptic copper complexes,light-emitting electrochemical cells,thermally activated delayed fluorescence,Phosphane tuning
更新于2025-09-19 17:15:36
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Luminescent Cyclic Trinuclear Coinage Metal Complexes with Aggregation-Induced Emission (AIE) Performance
摘要： A series of AIE active cyclic trinuclear complexes (Au3, Ag3, and Cu3) have been successfully prepared and elucidated by X-ray crystallography. These complexes showed excellent AIE properties and their quantum yields (QYs) were significantly increased compared to that of the free ligands. The remarkable solution induced AIE activity in atom-precise coinage metal complexes is still scarce, and this work opens a promising avenue for the development of easily prepared metal-based AIE luminogens with high emission efficiency.
关键词： Aggregation-Induced Emission,X-ray Crystallography,Quantum Yields,Coinage Metal Complexes,Luminescence
更新于2025-09-19 17:15:36
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Four-membered red iridium( <scp>iii</scp> ) complexes with Ira??Sa??Ca??S structures for efficient organic light-emitting diodes
摘要： Three sulfur atom contained ligands (diphenylcarbamodithioate (dpdtc), di-p-tolylcarbamodithioate (medtc) and bis(4-(trifluoromethyl)phenyl)carbamodithioate (cf3dtc)) were prepared for three red iridium(III) complexes. All (tfmpqz)2Ir(dpdtc), (tfmpqz)2Ir(medtc) and (tfmpqz)2Ir(cf3dtc) complexes were synthesized rapidly at room temperature in 5 min with high yields owing to strong coordination ability between sulfur and iridium atoms, in which 4-(4-(trifluoromethyl)phenyl)quinazoline (tfmpqz) was used as main ligand. Three Ir(III) complexes show distinct PL emissions at the range of 617 - 629 nm with high phosphorescence quantum yields up to of 83%, respectively. With these complexes as dopants, the organic light-emitting devices (OLEDs) with the double-emissive-layer structure of ITO/ HATCN (hexaazatriphenylenehexacabonitrile, 5 nm)/ TAPC ((bis(4-(N,N-ditolylamino)phenyl)cyclohexane, 30 nm)/ Ir(III) complexes: TCTA (4,4',4''-tris(carbazol-9-yl)-triphenylamine) (12 wt%, 10 nm)/ Ir(III) complexes: 26DCzppy (2,6-bis-(3-(carbazol-9-yl)phenyl)pyridine) (12 wt%, 10 nm)/ TmPyPB (1,3,5-tri((3-pyridyl)-phen-3-yl)benzene, 30 nm)/ LiF (1 nm)/ Al (100 nm) achieved good performances. In particular, the device employing (tfmpqz)2Ir(cf3dtc) complex exhibits the champion performances with a maximum luminance of 30 740 cd m-2 and a maximum external quantum efficiency of 26.10%, respectively.
关键词： phosphorescence quantum yields,sulfur atom,iridium(III) complexes,external quantum efficiency,OLEDs
更新于2025-09-19 17:13:59
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High quantum yields generated by a multi-band quantum dot photocell
摘要： We perform the quantum yields in a multi-band quantum dot (QD) photocell via doping an intermediate band (IB) between the conduction band (CB) and valence band (VB). Under two different sub-band gap layouts, the output power has a prominent enhancement than the single-band gap photocell and the achieved peak photo-to-charge efficiency reaches to 74.9% as compared to the limit efficiency of 63.2% via the IB approach in the theoretical solar cell prototype. The achieved quantum yields reveal the potential to improve efficiency by some effective theoretical approaches in the QD-IB photocell.
关键词： photo-to-charge efficiency,Quantum yields,a multi-band quantum dot photocell
更新于2025-09-12 10:27:22