Universal Flexible Lamination Encapsulation Strategy toward Underwater-Operation Electroluminescence Devices.

A reliable encapsulation technology with scalability and flexibility is urgently needed for electroluminescence devices. Here, we developed a simple, robust, low-cost, and scalable flexible lamination encapsulation strategy with quantum-dot light-emitting diodes (QLEDs) as the model devices. Multilayered Parafilm combining with calcium oxide buffer was used for the lamination encapsulation. We successfully demonstrated that such a Parafilm Lami encapsulation (PLE) not only allowed excellent protection for QLEDs in air but endowed QLED outstanding waterproof performance. As a result, highly efficient and stable flexible waterproof QLEDs were realized based on this PLE, exhibiting maximum external quantum efficiency of ∼8% and long half-luminescence lifetime of over 1.5 h in water. We believe that there are not any obstacles to extending this encapsulation technology to other flexible flat-panel devices, such as organic/perovskite light-emitting diodes.

Using magneto-electroluminescence as a fingerprint to identify the spin polarization and spin-orbit coupling of magnetic nanoparticle doped polymer light emitting diodes.

The spin polarization and spin-orbit coupling (SOC) in polymer light emitting diodes (PLEDs) with the active layer doped with Fe3O4 nanoparticles (NPs) were identified through magneto-electroluminescence (MEL). By comparing the MEL characteristics such as linewidth and magnitude between PLEDs with and without Fe3O4 dopant, we confirmed the existence of spin polarization, but ruled out the existence of SOC. Although the spin polarization is positive to electroluminescence, the brightness-current characteristics suggested that the current efficiency of the doped PLED does not improve. We attributed it to the current leakage caused by the Fe3O4 NPs in the active layer. This work is beneficial for us to further understand the effect of magnetic nanoparticle doping on the dynamic behavior of excitons and polaron pairs in organic semiconductor devices.

Intersystem Crossing and Triplet Fusion in Singlet-Fission-Dominated Rubrene-Based OLEDs Under High Bias Current.

Singlet fission is usually the only reaction channel for excited states in rubrene-based organic light-emitting diodes (OLEDs) at ambient temperature. Intriguingly, we discover that triplet fusion (TF) and intersystem crossing (ISC) within rubrene-based devices begin at moderate and high current densities (j), respectively. Both processes enhance with decreasing temperature. This behavior is discovered by analyzing the magneto-electroluminescence curves of the devices. The j-dependent magneto-conductance, measured at ambient temperature indicates that spin mixing within polaron pairs that are generated by triplet-charge annihilation (TQA) causes the occurrence of ISC, while the high concentrations of triplets are responsible for generating TF. Additionally, the reduction in exciton formation and the elevated TQA with decreasing temperature may contribute to the enhanced ISC at low temperatures. This work provides considerable insight into the different mechanisms that occur when a high density of excited states exist in rubrene and reasonable reasons for the absence of EL efficiency roll-off in rubrene-based OLEDs.

Guest concentration, bias current, and temperature-dependent sign inversion of magneto-electroluminescence in thermally activated delayed fluorescence devices.

Non-emissive triplet excited states in devices that undergo thermally activated delayed fluorescence (TADF) can be up-converted to singlet excited states via reverse intersystem crossing (RISC), which leads to an enhanced electroluminescence efficiency. Exciton-based fluorescence devices always exhibit a positive magneto-electroluminescence (MEL) because intersystem crossing (ISC) can be suppressed effectively by an external magnetic field. Conversely, TADF devices should exhibit a negative MEL because RISC is suppressed by the external magnetic field. Intriguingly, we observed a positive MEL in TADF devices. Moreover, the sign of the MEL was either positive or negative, and depended on experimental conditions, including doping concentration, current density and temperature. The MEL observed from our TADF devices demonstrated that ISC in the host material and RISC in the guest material coexisted. These competing processes were affected by the experimental conditions, which led to the sign change of the MEL. This work gives important insight into the energy transfer processes and the evolution of excited states in TADF devices.

Magneto-conductance characteristics of trapped triplet-polaron and triplet-trapped polaron interactions in anthracene-based organic light emitting diodes.

The effects of a magnetic field on the dissociation of triplet excitons by free charges (TCI) are well understood. However, the magneto-conductance (MC) characteristics of trapped triplet-polaron interactions (TtPI) and triplet-trapped polaron interactions (TPtI) within organic light emitting diodes (OLEDs) are not well understood. We have studied these interactions in an anthracene-based OLED. The electroluminescence spectra, current-voltage characteristics and magneto-electroluminescence indicated that the anthracene layer contained many defects that could trap either triplet excitons or polarons, which led to TPtI and TtPI. The MC curves at low temperature exhibited a complex line shape, which indicated that intersystem crossing, TPtI, TtPI, and TCI occurred simultaneously in the device. The individual MC characteristics of TPtI and TtPI were extracted from temperature dependant MC curves by fitting them to three empirical Lorentzian functions and one non-Lorentzian function. The MC of TPtI exhibited a negative sign, while that of TtPI exhibited a positive one, with characteristic magnetic fields (B0) of ∼10.5 and ∼15 mT, respectively. Both processes were prominent below 150 K and weakened with increasing temperature. TPtI was neglected above 200 K, while TtPI was observed even at ambient temperature. These results add significant insight into the magnetic field effects on triplet-polaron interactions.

In situ investigation of energy transfer in hybrid organic/colloidal quantum dot light-emitting diodes via magneto-electroluminescence.

Energy transfer (ET) and charge injection (CI) in the hybrid organic/colloidal quantum dot light-emitting diodes (QD-LEDs) have been investigated by using magneto-electroluminescence (MEL) as an in situ tool. The feasibility and availability of MEL as an in situ tool were systematically demonstrated in the typical QD-LEDs based on CdSe-ZnS core-shell QDs. Our results suggest that the ET and CI processes can be well discerned by MEL measurements since these two processes exhibit distinct responses to the applied magnetic field. Through measurement of the MEL and current efficiency, we indicated that ET would be the main mechanism for light emission in the present hybrid QD-LEDs. This study strongly suggests that MEL could be a highly sensitive fingerprint for ET, which provides a facile and efficient method for the in situ investigation of fundamental processes in hybrid organic/colloidal QD-LEDs and other organic/inorganic composites.

Determining the Origin of Half-bandgap-voltage Electroluminescence in Bifunctional Rubrene/C60 Devices.

Lowering the driving voltage of organic light-emitting diodes (OLEDs) is an important approach to reduce their energy consumption. We have fabricated a series of bifunctional devices (OLEDs and photovoltaics) using rubrene and fullerene (C60) as the active layer, in which the electroluminescence threshold voltage(~1.1 V) was half the value of the bandgap of rubrene. Magneto-electroluminescence (MEL) response of planner heterojunction diodes exhibited a small increase in response to a low magnetic field strength (<20 mT); however, a very large decay was observed at a high magnetic field strength (>20 mT). When a hole-transport layer with a low mobility was included in these devices, the MEL response reversed in shape, and simultaneously, the EL threshold voltage became larger than the bandgap voltage. When bulk heterojunction device was examined, the amplitude of MEL curves presented an anomalous voltage-dependence. Following an analysis of the MEL responses of these devices, we proposed that the EL of half-bandgap-voltage device originated from bimolecular triplet-triplet annihilation in the rubrene film, rather than from singlet excitons that formed via an interface auger recombination. This work provides critical insight into the mechanisms of OLED emission and will help advance the applications of bifunctional devices.

The triplet-charge annihilation in copolymer-based organic light emitting diodes: through the "Scattering Channel" or the "Dissociation Channel"?

In organic semiconductors, the triplet-charge annihilation (TCA) is one of the most common excitonic interactions influencing the opto-electronic power conversion efficiency of the devices. However, it is still unclear whether the TCA reaction goes through the "Scattering Channel" or the "Dissociation Channel". In this work, by measuring the organic magneto-current (OMC) of the conjugated co-polymer poly[{9,9-dioctyl-2,7-divinylene-fluorenylene}-alt-co-{2-methoxy-5-(2-ethylhexyloxy)-1,4-phenyene}] (PFOPV)-based organic light-emitting diodes (OLEDs) containing both localized exciton (LE) and charge-transfer-complex (CT), it is found that (3)LE and (3)CT play a crucial role in the "Scattering Channel" and the "Dissociation Channel" of TCA, respectively. This argument was supported by the simulations of Lorentzian and non-Lorentzian functions used, respectively, for intersystem crossing (or reverse intersystem crossing, RISC) and TCA effects. Moreover, by inserting a tris(2,4,6-trimethyl-3-(pyridin-3-yl)phenyl)borane (3TPYMB) layer between PFOPV and the cathode, we improved the electroluminescence efficiency of PFOPV-based OLEDs by suppressing the TCA when (3)CT involves in RISC. Our results give insights into the spin-dependent TCA limiting the efficiency of hotly discussed CT-based OLEDs.