Pengfei Yan

Ternary ambipolar phosphine oxide hosts based on indirect linkage for highly efficient blue electrophosphorescence: towards high triplet energy, low driving voltage and stable efficiencies.

The effective strategy of indirect linakge for constructing ternary ambipolar phosphine oxide (PO) hosts with the high first triplet energy levels (T(1)) was successfully demonstrated. The interplay between the chromophore, hole and electron transporting moieties was effectively restrained. Both of T(1) as high as 3.0 eV and ambipolar characteristics were perfectly realized, which consequently resulted in the highly efficient blue-emitting phosphorescent organic light-emitting diodes with low driving voltage and stable efficiencies.

A New Phosphine Oxide Host based on ortho‐Disubstituted Dibenzofuran for Efficient Electrophosphorescence: Towards High Triplet State Excited Levels and Excellent Thermal, Morphological and Efficiency Stability

An efficient host for blue and green electrophosphorescence, 4,6-bis(diphenylphosphoryl)dibenzofuran (o-DBFDPO), with the structure of a short-axis-substituted dibenzofuran was designed and synthesised. It appears that the greater density of the diphenylphosphine oxide (DPPO) moieties in the short-axis substitution configuration effectively restrains the intermolecular interactions, because only very weak π-π stacking interactions could be observed, with a centroid-to-centroid distance of 3.960 Å. The improved thermal stability of o-DBFDPO was corroborated by its very high glass transition temperature (T(g)) of 191 °C, which is the result of the symmetric disubstitution structure. Photophysical investigation showed o-DBFDPO to be superior to the monosubstituted derivative, with a longer lifetime (1.95 ns) and a higher photoluminescent quantum efficiency (61 %). The lower first singlet state excited level (3.63 eV) of o-DBFDPO demonstrates the stronger polarisation effect attributable to the greater number of DPPO moieties. Simultaneously, an extremely high first triplet state excited level (T(1)) of 3.16 eV is observed, demonstrating the tiny influence of short-axis substitution on T(1). The improved carrier injection ability, which contributed to low driving voltages of blue- and green-emitting phosphorescent organic light-emitting diodes (PHOLEDs), was further confirmed by Gaussian calculation. Furthermore, the better thermal and morphological properties of o-DBFDPO and the matched frontier molecular orbital (FMO) levels in the devices significantly reduced efficiency roll-offs. Efficient blue and green electrophosphorescence based on the o-DBFDPO host was demonstrated.

Convergent modulation of singlet and triplet excited states of phosphine-oxide hosts through the management of molecular structure and functional-group linkages for low-voltage-driven electrophosphorescence.

The controllable tuning of the excited states in a series of phosphine-oxide hosts (DPExPOCzn) was realized through introducing carbazolyl and diphenylphosphine-oxide (DPPO) moieties to adjust the frontier molecular orbitals, molecular rigidity, and the location of the triplet excited states by suppressing the intramolecular interplay of the combined multi-insulating and meso linkage. On increasing the number of substituents, simultaneous lowering of the first singlet energy levels (S(1)) and raising of the first triplet energy levels (T(1), about 3.0 eV) were achieved. The former change was mainly due to the contribution of the carbazolyl group to the HOMOs and the extended conjugation. The latter change was due to an enhanced molecular rigidity and the shift of the T(1) states from the diphenylether group to the carbazolyl moieties. This kind of convergent modulation of excited states not only facilitates the exothermic energy transfer to the dopants in phosphorescent organic light-emitting diodes (PHOLEDs), but also realizes the fine-tuning of electrical properties to achieve the balanced carrier injection and transportation in the emitting layers. As the result, the favorable performance of blue-light-emitting PHOLEDs was demonstrated, including much-lower driving voltages of 2.6 V for onset and 3.0 V at 100 cd m(-2), as well as a remarkably improved E.Q.E. of 12.6%.

An effective strategy for small molecular solution-processable iridium(III) complexes with ambipolar characteristics: towards efficient electrophosphorescence and reduced efficiency roll-off

A series of electrophosphorescent small molecular Ir3+ complexes IrPBIO22, IrPBICO, IrPBIO44 and IrPBIC22O22 for solution-processable host-free organic light-emitting diodes (OLEDs) were designed and synthesized, in which the electron-transporting 1,3,4-oxadiazole (OXD) and hole-transporting carbazole moieties were introduced through aliphatic chains to achieve balanced carrier injection/transporting. The coordinatable OXD groups were successfully and conveniently introduced through the post-substitution of Ir3+ cores. The photophysical investigation showed that compared with the single-position substituted counterparts, the double-position substitution is superior in restraining the quenching effect in solid states to endow the corresponding complexes with the much higher photoluminescence quantum yield (PLQY) in the film. The influences of peripheral carrier transporting (CT) moieties on the energy levels of frontier molecular orbitals were investigated with UPS analysis and Density Function Theory calculation. The dramatic electroluminescent (EL) performance of IrPBIC22O22 based on its host-free spin-coat phosphorescent organic light-emitting diodes (PHOLEDs), especially the remarkably restrained efficiency roll-off less than 16% at 1000 cd m−2 was realized, which demonstrated that the combined modification of the effective segregation of emitting cores by multi-position encapsulation and the balanced carrier injection/transporting through bipolar substitution is an effective strategy for realizing high-efficiency small molecular electrophosphorescent materials with the features of solution processability and strong restraining effect on quenching for host-free devices.

Solution-processible brilliantly luminescent Eu(III) complexes with host-featured phosphine oxide ligands for monochromic red-light-emitting diodes.

A series of solution-processible electroluminescent (EL) Eu(3+) complexes were constructed with a self-host strategy, in which neutral ligands were employed as functionalized bidentate phosphine oxide (PO) ligands named DPEPOArn (DPEPO = bis(2-(diphenylphosphino)phenyl) ether oxide). The solubility of these complexes was dramatically improved owing to the increased ratios of organic components. This further enhanced the antenna effect of these ligands in both singlet and triplet energy-transfer processes to support high photoluminescent quantum yields (PLQYs) up to 86 % for their Eu(3+) complexes, which is outstanding among conjugated Eu(3+) complexes. Density function theory (DFT) simulations and electrochemical analysis further verified the contributions of DPEPOArn to the carrier injecting/transporting ability of the complexes. In this sense, these functionalized PO ligands served as hosts in optoelectronic processes, which rendered the self-host feature of their Eu(3+) complexes. With the enhanced electrical properties, the spin-coated single-layer organic light-emitting diodes (OLEDs) of these complexes achieved improved low driving voltages, such as onset voltages about 6 V, compared to their Eu(3+)-contained red-emitting polymeric analogues. [Eu(DBM)3DPEPODPNA2] (DBM = 1,3-diphenylpropane-1,3-dione, DPNA = diphenylnaphthylamine) with the most enhanced electrical properties and suitable frontier molecular orbital (FMO) and triplet state locations endowed its devices with the biggest maximum luminance of >90 cd m(-2) and the highest EL efficiencies. This work verified the potential of small molecular EL Eu(3+) complexes for solution-processed OLEDs through rational function integrations.