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1.
Nanoscale Adv ; 3(20): 5900-5907, 2021 Oct 12.
Article in English | MEDLINE | ID: mdl-36132666

ABSTRACT

The effect of adding polyethylenimine (PEI) into the ZnO electron transport layer (ETL) of inverted quantum dot (QD) light emitting devices (QDLEDs) to form a blended ZnO:PEI ETL instead of using it in a separate layer in a bilayer ZnO/PEI ETL is investigated. Results show that while both ZnO/PEI bilayer ETL and ZnO:PEI blended ETL can improve device efficiency by more than 50% compared to QDLEDs with only ZnO, the ZnO:PEI ETL significantly improves device stability, leading to more than 10 times longer device lifetime. Investigations using devices with marking luminescent layers, electron-only devices and delayed electroluminescence measurements show that the ZnO:PEI ETL leads to a deeper penetration of electrons into the hole transport layer (HTL) of the QDLEDs. The results suggest that the stability enhancement may be due to a consequent reduction in hole accumulation at the QD/HTL interface. The findings show that ZnO:PEI ETLs can be used for enhancing both the efficiency and stability of QDLEDs. They also provide new insights into the importance of managing charge distribution in the charge transport layers for realizing high stability QDLEDs and new approaches to achieve that.

2.
Adv Sci (Weinh) ; 5(2): 1700608, 2018 02.
Article in English | MEDLINE | ID: mdl-29610726

ABSTRACT

A new concept of host, electroplex host, is developed for high efficiency and long lifetime phosphorescent organic light-emitting diodes by mixing two host materials generating an electroplex under an electric field. A carbazole-type host and a triazine-type host are selected as the host materials to form the electroplex host. The electroplex host is found to induce light emission through an energy transfer process rather than charge trapping, and universally improves the lifetime of red, yellow, green, and blue phosphorescent organic light-emitting diodes by more than four times. Furthermore, the electroplex host shows much longer lifetime than a common exciplex host. This is the first demonstration of using the electroplex as the host of high efficiency and long lifetime phosphorescent organic light-emitting diodes.

3.
J Am Chem Soc ; 140(20): 6260-6270, 2018 05 23.
Article in English | MEDLINE | ID: mdl-29688006

ABSTRACT

The pyren-1'-yl-functionalized dithiadiazolyl (DTDA) radical, C16H9CNSSN (1), is monomeric in solution and exhibits fluorescence in the deep-blue region of the visible spectrum (440 nm) upon excitation at 241 nm. The salt [1][GaCl4] exhibits similar emission, reflecting the largely spectator nature of the radical in the fluorescence process, although the presence of the radical leads to a modest quenching of emission (ΦF = 98% for 1+ and 50% for 1) through enhancement of non-radiative decay processes. Time-dependent density functional theory studies on 1 coupled with the similar emission profiles of both 1+ and 1 are consistent with the initial excitation being of predominantly pyrene π-π* character. Spectroscopic studies indicate stabilization of the excited state in polar media, with the fluorescence lifetime for 1 (τ = 5 ns) indicative of a short-lived excited state. Comparative studies between the energies of the frontier orbitals of pyren-1'-yl nitronyl nitroxide (2, which is not fluorescent) and 1 reveal that the energy mismatch and poor spatial overlap between the DTDA radical SOMO and the pyrene π manifold in 1 efficiently inhibit the non-radiative electron-electron exchange relaxation pathway previously described for 2. Solid-state films of both 1 and [1][GaCl4] exhibit broad emission bands at 509 and 545 nm, respectively. Incorporation of 1 within a host matrix for OLED fabrication revealed electroluminescence, with CIE coordinates of (0.205, 0.280) corresponding to a sky-blue emission. The brightness of the device reached 1934 cd/m2 at an applied voltage of 16 V. The crystal structure of 1 reveals a distorted π-stacked motif with almost regular distances between the pyrene rings but alternating long-short contacts between DTDA radicals. Solid state measurements on a thin film of 1 reveal emission occurs at shorter wavelengths (375 nm) whereas conductivity measurements on a single crystal of 1 show a photoconducting response at longer wavelength excitation (455 nm).

4.
ACS Appl Mater Interfaces ; 9(16): 14145-14152, 2017 Apr 26.
Article in English | MEDLINE | ID: mdl-28361540

ABSTRACT

We investigate the origins of the long-wavelength bands that appear in the emission spectra of carbazole-based host materials and play a role in the electroluminescence (EL) spectral changes of phosphorescent organic light emitting devices (PhOLEDs) with electrical aging. 4,4'-Bis(carbazol-9-yl)biphenyl (CBP) is used as a model carbazole host material and is studied using photoluminescence, EL, and atomic force microscopy measurements under various stress scenarios in both single and bilayer devices and in combination with various electron transport layer (ETL) materials. Results show that exciton-induced morphological aggregation of CBP is behind the appearance of those long-wavelength bands and that complexation between the aggregated CBP molecules and ETL molecules plays a role in this phenomenon. Comparisons between the effects of exciton and thermal stress suggest that exciton-induced aggregation may be limited to short-range molecular ordering or pairing (e.g., dimer or trimer species formation) versus longer-range ordering (crystallization) in the case of thermal stress. The findings provide new insights into exciton-induced degradation in wide band gap host materials and its role in limiting the stability of PhOLEDs.

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