Covalent organic frameworks (COFs) are an emerging class of highly tuneable crystalline, porous materials. Here we report the first COFs that change their electronic structure reversibly depending on ...the surrounding atmosphere. These COFs can act as solid-state supramolecular solvatochromic sensors that show a strong colour change when exposed to humidity or solvent vapours, dependent on vapour concentration and solvent polarity. The excellent accessibility of the pores in vertically oriented films results in ultrafast response times below 200 ms, outperforming commercially available humidity sensors by more than an order of magnitude. Employing a solvatochromic COF film as a vapour-sensitive light filter, we demonstrate a fast humidity sensor with full reversibility and stability over at least 4000 cycles. Considering their immense chemical diversity and modular design, COFs with fine-tuned solvatochromic properties could broaden the range of possible applications for these materials in sensing and optoelectronics.
The use of hybrid organic–inorganic perovskites in optoelectronic applications are attracting an interest because of their outstanding characteristics, which enable a remarkable enhancement of device ...efficiency. However, solution-processed perovskite crystals unavoidably contain defect sites that cause hysteresis in perovskite solar cells (PeSCs) and blinking in perovskite light-emitting diodes (PeLEDs). Here, we report significant beneficial effects using a new treatment based on amine-based passivating materials (APMs) to passivate the defect sites of methylammonium lead tribromide (MAPbBr3) through coordinate bonding between the nitrogen atoms and undercoordinated lead ions. This treatment greatly enhanced the PeLED’s efficiency, with an external quantum efficiency (EQE) of 6.2%, enhanced photoluminescence (PL), a lower threshold for amplified spontaneous emission (ASE), a longer PL lifetime, and enhanced device stability. Using confocal microscopy, we observed the cessation of PL blinking in perovskite films treated with ethylenediamine (EDA) due to passivation of the defect sites in the MAPbBr3.
Hybrid organic–inorganic perovskites allow the synthesis of high-quality, nanostructured semiconducting films via easily accessible solution-based techniques. This has allowed tremendous development ...in optoelectronic applications, primarily solar cells and light-emitting diodes. Allowed by the ease of access to nanostructure, chirality has recently been introduced in semiconducting perovskites as a promising way to obtain advanced control of charge and spin and for developing circularly polarized light sources. Circular polarization of photoluminescence (CPL) is a powerful tool to probe the electronic structure of materials. However, CPL in chiral perovskites has been scarcely investigated, and a study in bulk thin films and at room temperature is still missing. In this work, we fabricate bromine-based chiral perovskites by using a bulky chiral organic cation mixed with CsBr, resulting in Ruddlesden–Popper perovskite thin films. We measure CPL on these films at room temperature and, by using unpolarized photoexcitation, we record a degree of circular polarization of photoluminescence in the order of 10–3 and provide a full spectral characterization of CPL. Our results show that chirality is imparted on the electronic structure of the semiconductor; we hypothesize that the excess in polarization of emitted light originates from the charge in the photogenerated Wannier exciton describing an orbit in a symmetry-broken environment. Furthermore, our experiments allow the direct measurement of the magnetic dipole moment of the optical transition, which we estimate to be ≥0.1 μ B . Finally, we discuss the implications of our findings on the development of chiral semiconducting perovskites as sources of circularly polarized light.
The use of diiodooctane as processing additive for construction of PCPDTBT:PCBM solar cells results in a profound change in photophysical behavior of this blend. In the improved morphology obtained ...with the additive, recombination of charge carriers to the lowest triplet excited state is suppressed. This contributes to the boost in solar power conversion efficiency induced by the use of the processing agent.
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► In-depth study of the role of PEDOT:PSS in organic solar cell degradation in air. ► Separate investigation of the anode and cathode interfaces. ► Investigation of PEDOT:PSS acidic ...and hygroscopic nature on degradation. ► More than 10-fold lifetime enhancement with MoO
3 compared to PEDOT:PSS. ► Quantitative relationship between device lifetime and ambient humidity.
In this paper, we elucidate the role of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) in the degradation of polymer:PCBM ((6,6)-phenyl C
61-butyric acid methyl ester) solar cells. The study is done on unencapsulated cells exposed to ambient conditions in dark. The cell degradation results from reduced carrier extraction, and an investigation of the various interfaces within the cell allows us to correlate this to oxidation of the low work function metal cathode. We further show that this oxidation is caused by water vapor diffusion from the edges through the hygroscopic PEDOT:PSS layer. We demonstrate that only the hygroscopic nature of PEDOT:PSS, and not its acidity, has a detrimental impact. The oxidation of the cathode progresses in synchrony with the water ingress into the PEDOT:PSS layer from the edges of the device towards the central part, and results in a progressive constriction of the active area. When the PEDOT:PSS layer is replaced by an evaporated layer of MoO
3, the device lifetime is improved considerably even with highly reactive metal cathodes. Finally, we provide a quantitative relationship between device lifetime and the level of humidity in the ambient, thus establishing a suitable accelerated shelf-life test for organic solar cells and their encapsulation.
Organic–inorganic hybrid perovskites are emerging as promising emitting materials due to their narrow full-width at half-maximum emissions, color tunability, and high photoluminescence quantum yields ...(PLQYs). However, the thermal generation of free charges at room temperature results in a low radiative recombination rate and an excitation-intensity-dependent PLQY, which is associated with the trap density. Here, we report perovskite films composed of uniform nanosized single crystals (average diameter = 31.7 nm) produced by introducing bulky amine ligands and performing the growth at a lower temperature. By effectively controlling the crystal growth, we maximized the radiative bimolecular recombination yield by reducing the trap density and spatially confining the charges. Finally, highly bright and efficient green emissive perovskite light-emitting diodes that do not suffer from electroluminescence blinking were achieved with a luminance of up to 55 400 cd m–2, current efficiency of 55.2 cd A–1, and external quantum efficiency of 12.1%.
A perovskite LED with a perovskite film treated under optimum thermal annealing conditions exhibits a significantly enhanced long‐term stability with full coverage of the green electroluminescence ...emission due to the highly uniform morphology of the perovskite film.
Self-assembled helical polymers hold great promise as new functional materials, where helical handedness controls useful properties such as circularly polarized light emission or electron spin. The ...technique of subcomponent self-assembly can generate helical polymers from readily prepared monomers. Here we present three distinct strategies for chiral induction in double-helical metallopolymers prepared via subcomponent self-assembly: (1) employing an enantiopure monomer, (2) polymerization in a chiral solvent, (3) using an enantiopure initiating group. Kinetic and thermodynamic models were developed to describe the polymer growth mechanisms and quantify the strength of chiral induction, respectively. We found the degree of chiral induction to vary as a function of polymer length. Ordered, rod-like aggregates more than 70 nm long were also observed in the solid state. Our findings provide a basis to choose the most suitable method of chiral induction based on length, regiochemical, and stereochemical requirements, allowing stereochemical control to be established in easily accessible ways.
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