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1.
Beilstein J Org Chem ; 18: 1311-1321, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36225727

RESUMO

We designed and synthesized two new ionic thermally activated delayed fluorescent (TADF) emitters that are charged analogues of a known multiresonant TADF (MR-TADF) compound, DiKTa. The emission of the charged derivatives is red-shifted compared to the parent compound. For instance, DiKTa-OBuIm emits in the green (λPL = 499 nm, 1 wt % in mCP) while DiKTa-DPA-OBuIm emits in the red (λPL = 577 nm, 1 wt % in mCP). In 1 wt % mCP films, both emitters showed good photoluminescence quantum yields of 71% and 61%, and delayed lifetimes of 316.6 µs and 241.7 µs, respectively, for DiKTa-OBuIm and DiKTa-DPA-OBuIm, leading to reverse intersystem crossing rates of 2.85 × 103 s-1 and 3.04 × 103 s-1. Light-emitting electrochemical cells were prepared using both DiKTa-OBuIm and DiKTa-DPA-OBuIm as active emitters showing green (λmax = 534 nm) and red (λmax = 656 nm) emission, respectively.

2.
Photochem Photobiol Sci ; 18(9): 2180-2190, 2019 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-30816403

RESUMO

The one-photon (1P) and two-photon (2P) absorption properties of three quadrupolar dyes, featuring thiophene as a donor and acceptors of varying strengths, are determined by a combination of experimental and computational methods employing the density functional theory (DFT). The emission shifts in different solvents are well reproduced by time-dependent DFT calculations with the linear response and state specific approaches in the framework of the polarizable continuum model. The calculations show that the energies of both 1P- and 2P-active states decrease with an increase of the strength of the acceptor. The 2P absorption cross-sections predicted by the response theory are accounted for by considering just one intermediate state (S1) in the sum-over-states formulation. For the chromophore featuring the stronger acceptor, the energetic positions of the 1P- and 2P-active states prevent the exploitation of the theoretically predicted very high 2P activity due to the competing 1P absorption into the S1 state.

3.
ACS Photonics ; 9(7): 2483-2488, 2022 Jul 20.
Artigo em Inglês | MEDLINE | ID: mdl-35880074

RESUMO

Metal halide perovskites have emerged as a promising group of materials for optoelectronic applications such as photovoltaics, light emission, and photodetectors. So-far, in particular, the stability of light-emitting devices is limited, which is in part attributed to the intrinsic ionic conductivity of these materials. High-performance devices inevitably contain heterojunctions similar to other optoelectronic devices based on oxide perovskites, II-VI, or III-V group semiconductors. To enable efficient heterojunctions, ion exchange at the interface between different layers should be controlled. Herein, we report a method that enables to control and monitor the extent of anion intermixing between solution-processed lead bromide and vacuum-deposited lead chloride perovskite films. Taking advantage of the ability to fine tune the layer thicknesses of the vacuum-deposited films, we systematically study the effect of film thickness on anionic intermixing. Using these multiple layers, we prepare proof of principle light-emitting devices exhibiting green and blue electroluminescence.

4.
Dalton Trans ; 50(48): 17920-17934, 2021 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-34757348

RESUMO

The syntheses and characterisations of a series of heteroleptic copper(I) compounds [Cu(POP)(Mebpy)][A], [Cu(POP)(Me2bpy)][A], [Cu(xantphos)(Mebpy)][A] and [Cu(xantphos)(Me2bpy)][A] in which [A]- is [BF4]-, [PF6]-, [BPh4]- and [BArF4]- (Mebpy = 6-methyl-2,2'-bipyridine, Me2bpy = 6,6'-dimethyl-2,2'-bipyridine, POP = oxydi(2,1-phenylene)bis(diphenylphosphane), xantphos = (9,9-dimethyl-9H-xanthene-4,5-diyl)bis(diphenylphosphane), [BArF4]- = tetrakis(3,5-bis(trifluoromethyl)phenyl)borate) are reported. Nine of the compounds have been characterised by single crystal X-ray crystallography, and the consequences of the different anions on the packing interactions in the solid state are discussed. The effects of the counterion on the photophysical properties of [Cu(POP)(N^N)][A] and [Cu(xantphos)(N^N)][A] (N^N = Mebpy and Me2bpy) have been investigated. In the solid-state emission spectra, the highest energy emission maxima are for [Cu(xantphos)(Mebpy)][BPh4] and [Cu(xantphos)(Me2bpy)][BPh4] (λemmax = 520 nm) whereas the lowest energy λemmax values occur for [Cu(POP)(Mebpy)][PF6] and [Cu(POP)(Mebpy)][BPh4] (565 nm and 563 nm, respectively). Photoluminescence quantum yields (PLQYs) are noticeably affected by the counterion; in the [Cu(xantphos)(Me2bpy)][A] series, solid-state PLQY values decrease from 62% for [PF6]-, to 44%, 35% and 27% for [BF4]-, [BPh4]- and [BArF4]-, respectively. This latter series of compounds was used as active electroluminescent materials on light-emitting electrochemical cells (LECs). The luminophores were mixed with ionic liquids (ILs) [EMIM][A] ([EMIM]+ = [1-ethyl-3-methylimidazolium]+) containing the same or different counterions than the copper(I) complex. LECs containing [Cu(xantphos)(Me2bpy)][BPh4] and [Cu(xantphos)(Me2bpy)][BArF4] failed to turn on under the LEC operating conditions, whereas those with the smaller [PF6]- or [BF4]- counterions had rapid turn-on times and exhibited maximum luminances of 173 and 137 cd m-2 and current efficiencies of 3.5 and 2.6 cd A-1, respectively, when the IL contained the same counterion as the luminophore. Mixing the counterions ([PF6]- and [BF4]-) of the active complex and the IL led to a reduction in all the figures of merit of the LECs.

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