arXiv subjects

Joan Ràfols-Ribé

Publications and source records attributed to Joan Ràfols-Ribé.

6 recordsLinked to original sources

arXiv2026

Modifying Electrochemical Doping in Light-Emitting Electrochemical Cells with Gold Nanoparticles

Electrochemical doping offers dynamic control of the electronic properties of organic semiconductors, and it is the enabling feature of a range of technologies, including electrochemical transistors, energy-storage devices, light-emitting electrochemical cells (LECs), and bioelectronics. Electrochemical doping is commonly controlled by the selection of the constituents in the active material of the device or the applied voltage bias, but herein we report that the incorporation of Au nanoparticles (Au-NPs) at an electrode interface can constitute an alternative control parameter. The LEC features balanced p- and n-type electrochemical doping that forms a p-n junction doping structure in its active material, and we find that it is possible to reshape this doping profile by incorporating Au-NPs at an electrode interface. Specifically, we establish that the inclusion of neat non-capped Au-NPs at the anodic interface shifts the p-n junction (i.e., the emission zone) away from the anode. In contrast, the inclusion of Au-NPs capped with sodium citrate is found to reverse this behavior, so that the emission zone is instead moved towards the anode. We utilize this control parameter to shift the emission zone towards a position of constructive (destructive) interference, as manifested in a strong increase (decrease) of the LEC emission efficiency. Our findings establish an interfacial strategy for modulating the spatial profile of electrochemical doping and tuning device performance without altering the chemistry of the active material, relying instead on the surface modification of one electrode. This approach is important because it provides a versatile and minimally invasive route to optimize electrochemical devices while preserving the intrinsic properties and formulation of the active material.

cond-mat.mtrl-sci↗

arXiv2026

Round-Robin Test of a Light-Emitting Electrochemical Cell: Establishing a Reference Protocol for Quality Research

Emerging technologies benefit from a jointly established reference protocol, which can lower the bar of entry for new researchers while serving as a calibration standard for established actors. The light-emitting electrochemical cell (LEC) combines electrochemistry and optoelectronics in an intricate manner, and it can by that enable sustainable and commercially relevant printing fabrication of emissive thin-film devices. However, LEC performance is sensitive to a range of material and processing parameters, which frequently results in inadequate, or even erroneous, device evaluation. With this in mind, we present herein a LEC reference protocol, which details the sourcing of materials and the procedures and parameters for robust device fabrication and operation. The protocol has been tested across nine international research groups, and the collected results from this interlaboratory round-robin test confirm that good LEC performance can be reproducibly obtained following our protocol. We also identify common pitfalls that can arise during LEC development, and present practical steps for attaining optimum LEC performance. We hope this reference protocol will improve the quality of future LEC research and serve as a guide for future researchers entering this vibrant field.

cond-mat.soft↗

arXiv2025

In-operando dipole orientation for bipolar injection from air-stable electrodes into organic semiconductors

Efficient charge-carrier injection from air-stable electrodes into organic semiconductors (OSCs) is essential for fabricating solution-processed organic optoelectronic devices under ambient conditions. Today, this is typically achieved by incorporating doped OSC interlayers, introducing self-assembled dipole monolayers, or adding mobile ions to the active material (AM). Here, we demonstrate an alternative approach that eliminates the need for additional injection layers or ionic additives. We achieve this by blending the dipolar compound TMPE-OH into the electroluminescent polymer Super Yellow (SY) and depositing this sole AM between two air-stable electrodes, forming a single-layer, dipole-doped OLED (D-OLED). By tracking its transient voltage-luminance response, performing impedance spectroscopy, and comparing these characteristics with two other single-layer device concepts, i.e. a neat-SY OLED without a dipolar compound and a light-emitting electrochemical cell (LEC) containing mobile ions, we can establish that the auxiliary dipoles in the D-OLED reorient under the applied driving voltage, enabling immediate luminance turn-on and lowering the injection barriers at both electrodes. Finally, we demonstrate that the D-OLED achieves current efficacies comparable to those of SY OLEDs incorporating dedicated injection layers or LECs. Our study establishes dipolar doping as a practical strategy for efficient bipolar charge injection from air-stable electrodes in solution-processed organic semiconductor devices.

cond-mat.mtrl-sci↗

arXiv2024

Impact of the electrode material on the performance of light-emitting electrochemical cells

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. We rationalize this finding by proposing that the ion concentration in the injection-facilitating EDLs depends on the offset between the electrode work function and the respective semiconductor orbital, which in turn influences the number of ions available for electrochemical doping and hence shifts the exciton generation zone. Further, we investigate the effects of the electrode selection on exciton losses to surface plasmon polaritons and discuss the impact of cavity effects on the exciton density. We conclude by showing that the measured electrode-dependent LEC luminance transients can be replicated by an optical model that considers these electrode-dependent effects to calculate the attained light outcoupling of the LEC stack. As such, our findings provide rational design criteria considering the electrode materials, the active-material thickness, and its composition in concert to achieve optimum LEC performance.

physics.optics↗

arXiv2017

Evidence of thermal transport anisotropy in stable glasses of vapour deposited organic molecules

Vapour-deposited organic glasses are currently in use in many optoelectronic devices. Their operation temperature is limited by the glass transition temperature of the organic layers and thermal management strategies become increasingly important to improve the lifetime of the device. Here we report the unusual finding that molecular orientation heavily influences heat flow propagation in glassy films of small molecule organic semiconductors. The thermal conductivity of vapour-deposited thin-film semiconductor glasses is anisotropic and controlled by the deposition temperature. We compare our data with extensive molecular dynamics simulations to disentangle the role of density and molecular orientation on heat propagation. Simulations do support the view that thermal transport along the backbone of the organic molecule is strongly preferred with respect to the perpendicular direction. This is due to the anisotropy of the molecular interaction strength that limit the transport of atomic vibrations. This approach could be used in future developments to implement small molecule glassy films in thermoelectric or other organic electronic devices.

cond-mat.mtrl-sci↗

arXiv2016

Relaxation dynamics of glasses along a wide stability and temperature range

While lot of measurements describe the relaxation dynamics of the liquid state, experimental data of the glass dynamics at high temperatures are much scarcer. We use ultrafast scanning calorimetry to expand the timescales of the glass to much shorter values than previously achieved. Our data show that the relaxation time of glasses follows a super-Arrhenius behaviour in the high-temperature regime above the conventional devitrification temperature heating at 10 K/min. The liquid and glass states can be described by a common VFT-like expression that solely depends on temperature and limiting fictive temperature. We apply this common description to nearly-isotropic glasses of indomethacin, toluene and to recent data on metallic glasses. We also show that the dynamics of indomethacin glasses obey density scaling laws originally derived for the liquid. This work provides a strong connection between the dynamics of the equilibrium supercooled liquid and non-equilibrium glassy states.

cond-mat.soft↗