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The synthesis of carbon dots (CDs) with tailored properties commonly requires time-consuming trial-and-error experimentation, in part because of a poorly understood and controlled chemical conversion of the precursor material. Here, we first report on the solid-state pyrolysis or solvothermal conversion of an ortho-aminophenol (oAP) precursor, comprising ortho-disposed amino and hydroxyl groups on a benzene ring. We find that both conversion reactions resulted in a two emission-colour product, which could be separated into distinct blue-emitting CDs (bCDs, λpeak = 420 nm) and yellow-emitting CDs (yCDs, λpeak = 565 nm) by repetitive column chromatography. Systematic characterization revealed that both CDs comprise a planar graphene-like interior, but that they are distinguished by that the bCDs comprise an intermixed significant amino-rich fluorophore while the yCDs instead comprise a pyridinic-rich fluorophore. This implies that the bCDs are formed via activation of the amino group of the oAP precursor, whereas the synthesis of the yCDs constituted a simultaneous activation of both the amino and hydroxyl groups. With this knowledge at hand, we managed to direct the chemical conversion of the oAP precursor to yield either solely bCDs or yCDs by adding a catalyst (either the Lewis acid AlCl3·6H2O or the Lewis base NaOH) that selectively and efficiently activated only one of the reaction pathways. This demonstration is important in that it shows that the synthesis of CDs with desired properties can be realized with efficient rational instead of trial-and-error means.

Deep-blue (DB) emitters that feature high photoluminescence quantum yield (PLQY) and narrow spectral bandwidth are desired for a variety of optoelectronic applications, particularly for lighting, illumination, and lasing. Currently favored DB emitters constitute quantum dots comprising cadmium or lead and organic compounds derived from petroleum, but they suffer from toxicity and sustainability issues. Here, we report the solvothermal synthesis of DB-emitting carbon dots (DB-CDs) using bioderivable phloroglucinol as the sole starting material, which exhibit a peak emission wavelength of 403 nm, narrow spectral full width at half-maximum of 35 nm, and high PLQY of 61% in ethanol. The DB-CDs with a planar structure are demonstrated to comprise distinct graphene segments in a polyether-cross-link network, with the former functioning as the fluorophore. The application merit of the DB-CDs is exemplified by their implementation as the gain medium in a random laser device, which exhibits a threshold optical power density of 40.5 kW cm-2. This study thus demonstrates a path toward efficient and sustainable deep-blue emitters, which can be exploited in practical applications.

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 we can replicate the measured luminance transients by an optical model which considers these electrode-dependent effects. 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.

The attainment of white emission from a light-emitting electrochemical cell (LEC) is important, since it enables illumination and facile color conversion from devices that can be cost-efficient and sustainable. However, a drawback with current white LECs is that they either employ non-sustainable metals as an emitter constituent or are intrinsically efficiency limited by that the emitter only converts singlet excitons to photons. Organic compounds that emit by thermally activated delayed fluorescence (TADF) can address these issues since they can harvest all excitons for light emission while being metal free. Here, we report on the first white LEC based on solely metal-free TADF emitters, as accomplished through careful tuning of the energy-transfer processes and the electrochemically formed doping structure in the single-layer active material. The designed TADF-LEC emits angle-invariant white light (color rendering index = 88) with an external quantum efficiency of 2.1 % at a luminance of 350 cd/m².

Solar collectors have the potential for significant climate change mitigation by substituting heat produced with fossil fuels. To achieve this, collectors with highly efficient solar absorbers are essential. Carbon nanotubes are highly absorbing, sustainable, cheap, and thermally stable, making them a promising material for solar absorbers. However, achieving a high solar absorptance and low thermal emittance (solar selectivity), while maintaining good thermal stability and scalability is challenging. Here, we present a selective coating based on multi-walled carbon nanotubes and silica (SiO₂). A water-based dispersion enabled by carboxyl functionalization of the carbon nanotubes (CNT_F) is spray coated on a stainless steel (SS) substrate and fixated with sol-gel dip coated silica. The SS/CNT_F/SiO₂ surface exhibits an optical selectivity dependent on CNTF area load and with 0.83 gCNT m⁻² a solar absorptance and thermal emittance of 0.94 and 0.40, respectively, is achieved. The coating also demonstrates excellent thermal stability, with an estimated lifetime of >25 years at working temperatures ≤222°C. All together, we show that by using scalable and cheap technology, concurrent with sustainable materials and a simple structural design, we can manufacture a coating that exhibits properties suitable for low-to-mid-temperature applications. Our study highlights the potential of carbon-based solar absorbers.

Carbon dots (CDs) are an emerging class of nanomaterials with attractive optical properties, which promise to enable a variety of applications. An important and timely question is whether CDs can become a functional and sustainable alternative to incumbent optical nanomaterials, notably inorganic quantum dots. Herein, the current CD literature is comprehensively reviewed as regards to their synthesis and function, with a focus on sustainability aspects. The study quantifies why it is attractive that CDs can be synthesized with biomass as the sole starting material and be free from toxic and precious metals and critical raw materials. It further describes and analyzes employed pretreatment, chemical-conversion, purification, and processing procedures, and highlights current issues with the usage of solvents, the energy and material efficiency, and the safety and waste management. It is specially shown that many reported synthesis and processing methods are concerningly wasteful with the utilization of non-sustainable solvents and energy. It is finally recommended that future studies should explicitly consider and discuss the environmental influence of the selected starting material, solvents, and generated byproducts, and that quantitative information on the required amounts of solvents, consumables, and energy should be provided to enable an evaluation of the presented methods in an upscaled sustainability context.

Understanding “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. Emerging light-emitting electrochemical cells (LECs) can be cost- and energy-efficiently fabricated by ambient-air printing by virtue of the in situ formation of a p-n junction doping structure. However, this in situ doping transformation renders a meaningful efficiency analysis challenging. Herein, a method for separation and quantification of major LEC loss factors, notably the outcoupling efficiency and exciton quenching, is presented. Specifically, the position of the emissive p-n junction in common singlet-exciton emitting LECs is measured to shift markedly with increasing current, and the influence of this shift on the outcoupling efficiency is quantified. It is further verified that the LEC-characteristic high electrochemical-doping concentration renders singlet-polaron quenching (SPQ) significant already at low drive current density, but also that SPQ increases super-linearly with increasing current, because of increasing polaron density in the p-n junction region. This results in that SPQ dominates singlet-singlet quenching for relevant current densities, and significantly contributes to the efficiency roll-off. This method for deciphering the LEC efficiency roll-off can contribute to a rational realization of all-printed LEC devices that are efficient at highluminance.

Multiresonant thermally activated delayed fluorescence (MR-TADF) emitters have been the focus of extensive design efforts as they are recognized to show bright, narrowband emission, which makes them very appealing for display applications. However, the planar geometry and relatively large singlet–triplet energy gap lead to, respectively, severe aggregation-caused quenching (ACQ) and slow reverse intersystem crossing (RISC). Here, a design strategy is proposed to address both issues. Two MR-TADF emitters triphenylphosphine oxide (TPPO)-tBu-DiKTa and triphenylamine (TPA)-tBu-DiKTa have been synthesized. Twisted ortho-substituted groups help increase the intermolecular distance and largely suppress the ACQ. In addition, the contributions from intermolecular charge transfer states in the case of TPA-tBu-DiKTa help to accelerate RISC. The organic light-emitting diodes (OLEDs) with TPPO-tBu-DiKTa and TPA-tBu-DiKTa exhibit high maximum external quantum efficiencies (EQEmax) of 24.4% and 31.0%, respectively. Notably, the device with 25 wt% TPA-tBu-DiKTa showed both high EQEmax of 28.0% and reduced efficiency roll-off (19.9% EQE at 1000 cd m−2) compared to the device with 5 wt% emitter (31.0% EQEmax and 11.0% EQE at 1000 cd m−2). The new emitters were also introduced into single-layer light-emitting electrochemical cells (LECs), equipped with air-stable electrodes. The LEC containing TPA-tBu-DiKTa dispersed at 0.5 wt% in a matrix comprising a mobility-balanced blend-host and an ionic liquid electrolyte delivered blue luminance with an EQEmax of 2.6% at 425 cd m−2. The high efficiencies of the OLEDs and LECs with TPA-tBu-DiKTa illustrate the potential for improving device performance when the DiKTa core is decorated with twisted bulky donors.

It is crucial to develop functional electronic materials that can be processed from green solvents to achieve environmentally sustainable and cost-efficient printing fabrication of organic electronic devices. Here, the design and cost-efficient synthesis of two hydrophilic and emissive conjugated polymers, TQ-OEG and TQ2F-OEG, are presented, which are rendered hydrophilic through the grafting of oligo(ethylene glycol) (OEG) solubilizing groups onto the thiophene-quinoxaline conjugated backbone and thereby can be processed from a water:ethanol solvent mixture. It is shown that the introduction of the OEG groups enables for a direct dissolution of salts by the neat polymer for the attainment of solid-state ion mobility. These properties are utilized for the design and development of light-emitting electrochemical cells (LECs), the active materials of which can be solution cast from a water:ethanol-based ink. It is specifically shown that such an LEC device, comprising an optimized blend of the TQ2F-OEG emitter and a Li salt as the active material positioned between two air-stabile electrodes, delivers deep-red emission (peak wavelength = 670 nm) with a radiance of 185 µW m⁻² at a low drive voltage of 2.3 V. This study contributes relevant information as to how polymers and LEC devices can be designed and fabricated to combine functionality with sustainability.