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The application of doping in semiconductors plays a major role in the high performances achieved to date in inorganic devices. In contrast, doping has yet to make such an impact in organic electronics. One organic device that does make extensive use of doping is the light-emitting electrochemical cell (LEC), where the presence of mobile ions enables dynamic doping, which enhances carrier injection and facilitates relatively large current densities. The mechanism and effects of doping in LECs are, however, still far from being fully understood, as evidenced by the existence of two competing models that seem physically distinct: the electrochemical doping model and the electrodynamic model. Both models are supported by experimental data and numerical modeling. Here, we show that these models are essentially limits of one master model, separated by different rates of carrier injection. For ohmic nonlimited injection, a dynamic p−n junction is formed, which is absent in injection-limited devices. This unification is demonstrated by both numerical calculations and measured surface potentials as well as light emission and doping profiles in operational devices. An analytical analysis yields an upper limit for the ratio of drift and diffusion currents, having major consequences on the maximum current density through this type of device.

Incorporation of ions in the active layer of organic semiconductor devices may lead to attractive device properties like enhanced injection and improved carrier transport. In this paper, we investigate the effect of the salt concentration on the operation of light-emitting electrochemical cells, using experiments and numerical calculations. The current density and light emission are shown to increase linearly with increasing ion concentration over a wide range of concentrations. The increasing current is accompanied by an ion redistribution, leading to a narrowing of the recombination zone. Hence, in absence of detrimental side reactions and doping-related luminescence quenching, the ion concentration should be as high as possible.

We demonstrate that the electrochemical properties of the electrode material can have a dramatic impact on the performance of light-emitting electrochemical cells (LECs). Specifically, we report results from planar wide-gap LECs containing a blend of poly(2-methoxy,5-(2’-ethylhexyloxy)-p-phenylene vinylene) (MEH-PPV), poly(ethylene oxide) and LiCF3SO3 as the active material. We find that Au electrodes are preferable over Al electrodes, since Au-electrode devices exhibit fast turn-on (i.e., p-n junction formation time) and clearly visible light emission during operation at 5 V and 360 K, while Al-electrode devices exhibit slow turn-on (due to a delayed onset of p-doping progression) and no visible light emission. These results are rationalized with a cyclic voltammetry study, which demonstrates that Al is oxidized at a lower potential than the p-doping (oxidation) potential of MEH-PPV, while Au is electrochemically inert over the entire voltage range spanned by the p- and n-doping potentials of MEH-PPV. Consequently, the oxidation charge injected into Al-electrode devices results in a combination of p-doping of MEH-PPV and formation of Al ions. The latter process is undesired since it results in a slow turn-on time and quenched light emission. Finally, we find that planar LECs in a bottom-electrode configuration exhibit a faster turn-on time than identical devices with the electrodes on top of the active material.

Polymer light-emitting electrochemical cells (LECs) offer an attractive opportunity for low-cost production of functional devices in flexible and large-area configurations, but the critical drawback in comparison to competing light-emission technologies is a limited operational lifetime. Here, it is demonstrated that it is possible to improve the lifetime by straightforward and motivated means from a typical value of a few hours to more than one month of uninterrupted operation at significant brightness (>100 cd m⁻²) and relatively high power conversion efficiency (2 lm W⁻¹ for orange-red emission). Specifically, by optimizing the composition of the active material and by employing an appropriate operational protocol, a desired doping structure is designed and detrimental chemical and electrochemical side reactions are identified and minimized. Moreover, the first functional flexible LEC with a similar promising device performance is demonstrated.

 We show that the electrochemical stability window of the constituent components in light-emitting electrochemical cells (LECs), e.g., the electrolyte, should be considered in order to minimize undesired side reactions. By designing and operating LECs in accordance with straightforward principles, we demonstrate sandwich cells that turn on fast at room temperature (<2 s), and which emit significant yellow-green light (>100 cd/m2) during 25 days of uninterrupted operation at low voltage (<4 V) and high power conversion efficacy ~6 lm/W. We further demonstrate that it is possible to attain balanced p- and n-type doping and a centered p-n junction in such planar LECs based on the conjugated polymer “superyellow.”

The current generation of polymer light-emitting electrochemical cells (LECs) suffers from insufficient stability during operation. One identified culprit is the active material, which comprises an intimate blend between an ion-conducting electrolyte and an electron-transporting conjugated polymer, as it tends to undergo phase separation during long-term operation and the intimate contact between the ion- and electron-transporting components provokes side reactions. To address these stability issues, we present here a bilayer LEC structure in which the electrolyte is spatially separated from the conjugated polymer. We demonstrate that employing this novel device structure, with its clearly separated ion- and electron-transport paths, leads to distinctly improved LEC performance in the form of decreased turn-on time and improved light emission. We also point out that it will allow for the utilization of combinations of active materials having mutually incompatible solubilities.

The emerging field of “organic” or “plastic” electronics has brought low-voltage, ultrathin, and energy-efficient lighting and displays to market as organic light-emitting diode (OLED) televisions and displays in cameras and mobile phones. Despite using carbon-based materials as the light-emitting layer, previous efficient organic electronic light-emitting devices have required at least one metal electrode. Here, we utilize chemically derived graphene for the transparent cathode in an all-plastic sandwich-structure device, similar to an OLED, called a light-emitting electrochemical cell (LEC). Using a screen-printable conducting polymer as a partially transparent anode and a micrometer-thick active layer solution-deposited from a blend of a light-emitting polymer and a polymer electrolyte, we demonstrate a light-emitting device based solely on solution-processable carbon-based materials. Our results demonstrate that low-voltage, inexpensive, and efficient light-emitting devices can be made without using metals. In other words, electronics can truly be “organic”.

We report flexible and metal-free light-emitting electrochemical cells (LECs) using exclusively solution-processed organic materials and illustrate interesting design opportunities offered by such conformable devices with transparent electrodes. Flexible LEC devices based on chemically derived graphene (CDG) as the cathode and poly(3,4-ethylenedioxythiophene) mixed with poly(styrenesulfonate) as the anode exhibit a low turn-on voltage for yellow light emission (V = 2.8 V) and a good efficiency 2.4 (4.0) cd/A at a brightness of 100 (50) cd/m². We also find that CDG is electrochemically inert over a wide potential range (+1.2 to −2.8 V vsferrocene/ferrocenium) and exploit this property to demonstrate planar LEC devices with CDG as both the anode and the cathode.