ACS Appl Mater Interfaces
January 2025
Light-emitting electrochemical cells (LECs) are promising candidates for fully solution-processed lighting applications because they can comprise a single active-material layer and air-stable electrodes. While their performance is often claimed to be independent of the electrode material selection due to the in situ formation of electric double layers (EDLs), we demonstrate conceptually and experimentally that this understanding needs to be modified. Specifically, the exciton generation zone is observed to be affected by the electrode work function.
View Article and Find Full Text PDFUnderstanding "efficiency roll-off" (i.e., the drop in emission efficiency with increasing current) is critical if efficient and bright emissive technologies are to be rationally designed.
View Article and Find Full Text PDFThe initial operation of a light-emitting electrochemical cell (LEC) constitutes the in-situ formation of a p-n junction doping structure in the active material by electrochemical doping. It has been firmly established that the spatial position of the emissive p-n junction in the interelectrode gap has a profound influence on the LEC performance because of exciton quenching and microcavity effects. Hence, practical strategies for a control of the position of the p-n junction in LEC devices are highly desired.
View Article and Find Full Text PDFThe concept of a metal-free and all-organic electroluminescent device is appealing from both sustainability and cost perspectives. Herein, we report the design and fabrication of such a light-emitting electrochemical cell (LEC), comprising a blend of an emissive semiconducting polymer and an ionic liquid as the active material sandwiched between two poly(3,4-ethylenedioxythiophene):poly(styrene-sulfonate) (PEDOT:PSS) conducting-polymer electrodes. In the off-state, this all-organic LEC is highly transparent, and in the on-state, it delivers uniform and fast to turn-on bright surface emission.
View Article and Find Full Text PDFThe position of the emission zone (EZ) in the active material of a light-emitting electrochemical cell (LEC) has a profound influence on its performance because of microcavity effects and doping- and electrode-induced quenching. Previous attempts of EZ control have focused on the two principal constituents in the active material-the organic semiconductor (OSC) and the mobile ions-but this study demonstrates that it is possible to effectively control the EZ position through the inclusion of an appropriate additive into the active material. More specifically, it is shown that a mere modification of the end group on an added neutral compound, which also functions as an ion transporter, results in a shifted EZ from close to the anode to the center of the active material, which translates into a 60% improvement of the power efficiency.
View Article and Find Full Text PDFThe emerging field of printed electronics uses large amounts of printing and coating solvents during fabrication, which commonly are deposited and evaporated within spaces available to workers. It is in this context unfortunate that many of the currently employed solvents are non-desirable from health, safety, or environmental perspectives. Here, we address this issue through the development of a tool for the straightforward identification of functional and "green" replacement solvents.
View Article and Find Full Text PDFThin film stable glasses transform into a liquid by a moving front that propagates from surfaces or interfaces with higher mobility. We use calorimetric data of vapor-deposited glasses of different thicknesses and stabilities to identify the role of glassy and liquid dynamics on the transformation process. By invoking the existence of an ultrathin intermediate layer whose transformation strongly depends on the properties of both the liquid and the glass, we show that the recovery to equilibrium is driven by the mismatch in the dynamics between glass and liquid.
View Article and Find Full Text PDFPhysical vapour deposition has emerged as the technique to obtain glasses of unbeatable stability. However, vapour deposited glasses exhibit a different transformation mechanism to ordinary glasses produced from liquid. Vapour deposited glasses of different thermodynamic stability, from ultrastable to those similar to ordinary glasses, transform into the liquid state via front propagation starting at the most mobile surfaces/interfaces, at least for the first stages of the transformation, eventually dynamiting the high thermal stability achieved for some of these glasses.
View Article and Find Full Text PDFOrganic light-emitting diodes (OLEDs) are one of the key solid-state light sources for various applications including small and large displays, automotive lighting, solid-state lighting, and signage. For any given commercial application, OLEDs need to perform at their best, which is judged by their device efficiency and operational stability. We present OLEDs that comprise functional layers fabricated as ultrastable glasses, which represent the thermodynamically most favorable and, thus, stable molecular conformation achievable nowadays in disordered solids.
View Article and Find Full Text PDFPhysical vapour deposition (PVD) has settled in as an alternative method to prepare glasses with significantly enhanced properties, providing new insights into the understanding of glass transition. One of the striking properties of some PVD glasses is their transformation into liquid via a heterogeneous mechanism that initiates at surfaces/interfaces. Here, we use membrane-based fast-scanning nanocalorimetry (10 K s) to analyse the variables that govern the transformation mechanism of vapour-deposited toluene glasses with different stabilities.
View Article and Find Full Text PDFWhile ordinary glasses transform into supercooled liquid via a homogeneous bulk mechanism, thin film glasses of higher stability transform heterogeneously by a front propagating from the surface and/or the interfaces. In this work, we use quasi-adiabatic fast scanning nanocalorimetry to determine the heat capacity of thin glassy layers of indomethacin vapor-deposited in a broad temperature range of 110 K below the glass transition temperature. Their variation in fictive temperature amounts to 40 K.
View Article and Find Full Text PDFUltrastable thin film glasses transform into supercooled liquid via propagating fronts starting from the surface and/or interfaces. In this paper, we analyze the consequences of this mechanism in the interpretation of specific heat curves of ultrastable glasses of indomethacin for samples with varying thickness from 20 nm up to several microns. We demonstrate that ultrastable films above 20 nm have identical fictive temperatures and that the apparent change of onset temperature in the specific heat curves originates from the mechanism of transformation and the normalization procedure.
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