Two efficient blue thermally activated delayed fluorescence compounds, B-oCz and B-oTC, composed of ortho-donor (D)-acceptor (A) arrangement were designed and synthesized. The significant intramolecular D-A interactions induce a combined charge transfer pathway and thus achieve small ΔE and high efficiencies. The concentration quenching can be effectively inhibited in films of these compounds. The blue non-doped organic light emitting diodes (OLEDs) based on B-oTC prepared from solution processes shows record-high external quantum efficiency (EQE) of 19.1 %.
In this communication, we report a new greenish-blue-emitting Cu(i) complex, Cu4Cl4(NP)2, a with high photoluminescence quantum yield of 90% and a short decay time of 9.9 μs. Due to the strong SOC combined with the small activation energy ΔEST, the emission at room temperature consists of approximately equivalent fast phosphorescence and TADF.
Herein, we present a new strategy in which highly emissive
thermally
activated delayed fluorescence (TADF) materials can be obtained from
modifying or tuning a non-TADF donor (D)–acceptor (A)-type
organic molecule via coordination of the metal ionic fragment. Theoretical
calculation and photophysical properties reveal that the D–A-type
free ligand emits both weak fluorescence and dual room-temperature
phosphorescence, whereas the two Ag(I) complexes display efficient
blue TADF, exhibiting photoluminescence quantum yields nearly 100%
in films with short decay lifetimes (τ ≈ 6 μs).
This is attributed to the four optimized parameters induced by Ag(I)
coordination: (1) narrow singlet (S1)–triplet (T1) energy gaps (ΔE
ST). (2)
T1 states have a hybrid local excitation and charge transfer
(CT) character, and S1 states have a predominant CT character.
Both the parameters facilitate reverse intersystem crossing. (3) Radiative
rate constant (k
r(S1→S0)) is increased.
(4) Molecular rigidity is strengthened. For the first time, this work
shows a powerful method to design efficient ligand-centered TADF in
Ag(I) complexes based on the conventional D–A-type molecule,
which significantly enriches the chemical space for the development
of TADF materials.
Room-temperature phosphorescence (RTP) was realized for the first time in a polyoxometalate-based charge-transfer (CT) hybrid material bearing polyoxometalates (POMs) as electron-donors (D) and rigid naphthalene diimides (NDIs) as electron-acceptors (A), meanwhile, this hybrid material displayed photochromism as well. The significant D-A anion-π interaction induced an additional through-space charge-transfer pathway. The resulting suitable D-A CT states can efficiently bridge the relatively large energy gap between the NDI-localized π-π* and π-π* states and thus trigger the ligand-localized phosphorescence ( π-π*).
Two mononuclear cuprous complexes [Cu(PNNA)(POP)]BF4 (1) and [Cu(PNNA)(Xantphos)]BF4 (2) (PNNA = 9,9-dimethyl-10-(6-(3-phenyl-1H-pyrazol-1-yl)pyridin-3-yl)-9,10-dihydroacridine, POP = bis[2-(dipenylphosphino)phenyl]ether, Xantphos =4,5-bis(diphenylphosphino)-9,9-dimethylxanthene), with intense bluish-green luminescence based on a new diimine ligand were designed and synthesized. Their structural, electrochemical, and photophysical properties were characterized by single-crystal X-ray analysis, cyclic voltammetry, temperature dependence of spectroscopy, time-dependent emission spectroscopy, etc. The complexes exhibit high photoluminescence quantum yields in doped films (up to 74.6%) at room temperature. Thermally activated delayed fluorescence based on intraligand charge transfer was observed by grafting a strong electron-donor moiety, 9,9-dimethylacridan, on the diimine ligand, which is supported by the density functional theory calculations on two complexes. Highly efficient solution-processed OLEDs based on these two complexes were fabricated, among which the electroluminescent device using 2 as dopant shows a peak external quantum efficiency of 7.42%, a peak current efficiency of 20.24 cd/A, and a maximum brightness of 5579 cd/m(2).
Metal‐free ultralong organic phosphorescence (UOP) materials have attracted significant attention owing to their anomalous photophysical properties and potential applications in various fields. Here, three pyrimidine‐based organic luminogens, 9‐(pyrimidin‐2‐yl)‐9H‐carbazole, 9‐(4,6‐dimethylpyrimidin‐2‐yl)‐9H‐carbazole, and 9‐(5‐bromopyrimidin‐2‐yl)‐9H‐carbazole are designed and synthesized, which show efficient yellow UOP with the longest lifetimes up to 1.37 s and the highest absolute phosphorescence quantum yields up to 23.6% under ambient conditions. Theoretical calculations, crystal structures, and photophysical properties of these compounds reveal that intramolecular hydrogen bonding, intermolecular π–π interactions, and intermolecular electronic coupling are responsible for forming dimers and generating highly efficient UOP. Their efficacy as solid materials for data encryption is demonstrated.
Strongly emissive copper(i) halide complexes constructed from a new tetradentate chelating ligand and butterfly-shaped Cu2X2 cores are presented and systematically investigated.
Two efficient blue thermally activated delayed fluorescence compounds, B‐oCz and B‐oTC, composed of ortho‐donor (D)–acceptor (A) arrangement were designed and synthesized. The significant intramolecular D–A interactions induce a combined charge transfer pathway and thus achieve small ΔEST and high efficiencies. The concentration quenching can be effectively inhibited in films of these compounds. The blue non‐doped organic light emitting diodes (OLEDs) based on B‐oTC prepared from solution processes shows record‐high external quantum efficiency (EQE) of 19.1 %.
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