High triplet energy host material with a 1,3,5-oxadiazine core from a one-step interrupted Fischer indolization.

Energy-efficient and deep-blue organic light-emitting diode (OLED) with long operating stability remains a key challenge to enable a disruptive change in OLED display and lighting technology. Part of the challenge is associated with a very narrow choice of the robust host materials having over 3 eV triplet energy level to facilitate efficient deep-blue emission and deliver excellent performance in the OLED device. Here we show the molecular design of new 1,3,5-oxadiazines (NON)-host materials with high triplet energy over 3.

The Interplay of Strongly and Weakly Exchange-Coupled Triplet Pairs in Intramolecular Singlet Fission.

Singlet fission (SF) and triplet-triplet annihilation upconversion (TTA-UC) nominally enable the interconversion of higher-energy singlet states with two lower-energy triplet states and vice versa, with both processes having envisaged application for enhanced solar power devices. The mechanism of SF/TTA-UC involves a complex array of different multiexcitonic triplet-pair states that are coupled by the exchange interaction to varying extents. In this work a family of bounded intramolecular SF materials, based upon the chromophore 1,6-diphenyl-1,3,5-hexatriene, were designed and synthesized.

Extending the defect tolerance of halide perovskite nanocrystals to hot carrier cooling dynamics.

Defect tolerance is a critical enabling factor for efficient lead-halide perovskite materials, but the current understanding is primarily on band-edge (cold) carriers, with significant debate over whether hot carriers can also exhibit defect tolerance. Here, this important gap in the field is addressed by investigating how intentionally-introduced traps affect hot carrier relaxation in CsPbX nanocrystals (X = Br, I, or mixture). Using femtosecond interband and intraband spectroscopy, along with energy-dependent photoluminescence measurements and kinetic modelling, it is found that hot carriers are not universally defect tolerant in CsPbX, but are strongly correlated to the defect tolerance of cold carriers, requiring shallow traps to be present (as in CsPbI).

Efficient near-infrared organic light-emitting diodes with emission from spin doublet excitons.

The development of luminescent organic radicals has resulted in materials with excellent optical properties for near-infrared emission. Applications of light generation in this range span from bioimaging to surveillance. Although the unpaired electron arrangements of radicals enable efficient radiative transitions within the doublet-spin manifold in organic light-emitting diodes, their performance is limited by non-radiative pathways introduced in electroluminescence.

Strong angular and spectral narrowing of electroluminescence in an integrated Tamm-plasmon-driven halide perovskite LED.

Next-generation light-emitting applications such as displays and optical communications require judicious control over emitted light, including intensity and angular dispersion. To date, this remains a challenge as conventional methods require cumbersome optics. Here, we report highly directional and enhanced electroluminescence from a solution-processed quasi-2-dimensional halide perovskite light-emitting diode by building a device architecture to exploit hybrid plasmonic-photonic Tamm plasmon modes.

Fabrication of red-emitting perovskite LEDs by stabilizing their octahedral structure.

Light-emitting diodes (LEDs) based on metal halide perovskites (PeLEDs) with high colour quality and facile solution processing are promising candidates for full-colour and high-definition displays. Despite the great success achieved in green PeLEDs with lead bromide perovskites, it is still challenging to realize pure-red (620-650 nm) LEDs using iodine-based counterparts, as they are constrained by the low intrinsic bandgap. Here we report efficient and colour-stable PeLEDs across the entire pure-red region, with a peak external quantum efficiency reaching 28.

Quantum barriers engineering toward radiative and stable perovskite photovoltaic devices.

Efficient photovoltaic devices must be efficient light emitters to reach the thermodynamic efficiency limit. Here, we present a promising prospect of perovskite photovoltaics as bright emitters by harnessing the significant benefits of photon recycling, which can be practically achieved by suppressing interfacial quenching. We have achieved radiative and stable perovskite photovoltaic devices by the design of a multiple quantum well structure with long (∼3 nm) organic spacers with oleylammonium molecules at perovskite top interfaces.

Deep-Blue and Fast Delayed Fluorescence from Carbene-Metal-Amides for Highly Efficient and Stable Organic Light-Emitting Diodes.

Linear gold complexes of the "carbene-metal-amide" (CMA) type are prepared with a rigid benzoguanidine amide donor and various carbene ligands. These complexes emit in the deep-blue range at 424 and 466 nm with 100% quantum yields in all media. The deep-blue thermally activates delayed fluorescence originates from a charge transfer state with an excited state lifetime as low as 213 ns, resulting in fast radiative rates of 4.

Understanding Spin-Triplet Excited States in Carbene-Metal-Amides.

Carbene-metal-amides (CMAs) are emerging delayed fluorescence materials for organic light-emitting diode (OLED) applications. CMAs possess fast, efficient emission owing to rapid forward and reverse intersystem crossing (ISC) rates. The resulting dynamic equilibrium between singlet and triplet spin manifolds distinguishes CMAs from most purely organic thermally activated delayed fluorescence emitters.

Identifying Current Collectors that Enable Light-Battery Interactions.

In recent years, there has been an increased focus on studying light-battery interactions in the context of operando optical studies and integrated photoelectrochemical energy harvesting. However, there has been little insight into identifying suitable "light-accepting" current collectors for this class of batteries. In this study, fluorine-doped tin oxide, indium-tin oxide, and silver nanowire-graphene films are analyzed along with carbon paper, carbon nanotube paper, and stainless-steel mesh as current collectors for optical batteries.

Excited-State Engineering Enables Efficient Deep-Blue Light-Emitting Diodes Exhibiting BT.2020 Color Gamut.

Organic luminescent materials that exhibit thermally activated delayed fluorescence (TADF) can convert non-emissive triplet excitons into emissive singlet states through a reverse intersystem crossing (RISC) process. Therefore, they have tremendous potential for applications in organic light-emitting diodes (OLEDs). However, with the development of ultra-high definition 4K/8K display technologies, designing efficient deep-blue TADF materials to achieve the Commission Internationale de l'Éclairage (CIE) coordinates fulfilling BT.

Suppression of Dexter transfer by covalent encapsulation for efficient matrix-free narrowband deep blue hyperfluorescent OLEDs.

Hyperfluorescence shows great promise for the next generation of commercially feasible blue organic light-emitting diodes, for which eliminating the Dexter transfer to terminal emitter triplet states is key to efficiency and stability. Current devices rely on high-gap matrices to prevent Dexter transfer, which unfortunately leads to overly complex devices from a fabrication standpoint. Here we introduce a molecular design where ultranarrowband blue emitters are covalently encapsulated by insulating alkylene straps.

Ligand-Directed Self-Assembly of Organic-Semiconductor/Quantum-Dot Blend Films Enables Efficient Triplet Exciton-Photon Conversion.

Blends comprising organic semiconductors and inorganic quantum dots (QDs) are relevant for many optoelectronic applications and devices. However, the individual components in organic-QD blends have a strong tendency to aggregate and phase-separate during film processing, compromising both their structural and electronic properties. Here, we demonstrate a QD surface engineering approach using electronically active, highly soluble semiconductor ligands that are matched to the organic semiconductor host material to achieve well-dispersed inorganic-organic blend films, as characterized by X-ray and neutron scattering, and electron microscopies.

Does Heat Play a Role in the Observed Behavior of Aqueous Photobatteries?

Light-rechargeable photobatteries have emerged as an elegant solution to address the intermittency of solar irradiation by harvesting and storing solar energy directly through a battery electrode. Recently, a number of compact two-electrode photobatteries have been proposed, showing increases in capacity and open-circuit voltage upon illumination. Here, we analyze the thermal contributions to this increase in capacity under galvanostatic and photocharging conditions in two promising photoactive cathode materials, VO and LiMnO.

Highly phosphorescent carbene-metal-carboranyl complexes of copper(I) and gold(I).

New phosphorescent "carbene-metal-carboranyl" (CMC) Cu(I) and Au(I) complexes based on the diamidocarbene (DAC) ligand show up to 68% photoluminescence quantum yield and microsecond range lifetimes. CMC organic light emitting diodes (OLEDs) emit sky-blue and warm white electroluminescence.

Phosphorescent Carbene-Gold-Arylacetylide Materials as Emitters for Near UV-OLEDs.

A series of carbene-gold-acetylide complexes [(BiCAAC)AuCC] C H (n = 1, Au1; n = 2, Au2; n = 3, Au3; BiCAAC = bicyclic(alkyl)(amino)carbene) have been synthesized in high yields. Compounds Au1-Au3 exhibit deep-blue to blue-green phosphorescence with good quantum yields up to 43% in all media. An increase of the (BiCAAC)Au moieties in gold complexes Au1-Au3 increases the extinction coefficients in the UV-vis spectra and stronger oscillator strength coefficients supported by theoretical calculations.

Thermalization and relaxation mediated by phonon management in tin-lead perovskites.

Understanding and control of ultrafast non-equilibrium processes in semiconductors is key to making use of the full photon energy before relaxation, leading to new ways to break efficiency limits for solar energy conversion. In this work, we demonstrate the observation and modulation of slow relaxation in uniformly mixed tin-lead perovskites (MASnPbI and CsSnPbI nanocrystals). Transient absorption measurements reveal that slow cooling mediated by a hot phonon bottleneck effect appears at carrier densities above ~10 cm for tin-lead alloy nanocrystals, and tin addition is found to give rise to suppressed cooling.

Spatially Resolved Optical Efficiency Measurements of Luminescent Solar Concentrators.

Luminescent solar concentrators (LSCs) are able to concentrate both direct and diffuse solar radiation, and this ability has led to great interest in using them to improve solar energy capture when coupled to traditional photovoltaics (PV). In principle, a large-area LSC could concentrate light onto a much smaller area of PV, thus reducing costs or enabling new architectures. However, LSCs suffer from various optical losses which are hard to quantify using simple measurements of power conversion efficiency.

Insights into the kinetics and self-assembly order of small-molecule organic semiconductor/quantum dot blends during blade coating.

Organic-inorganic nanocomposite films formed from blends of small-molecule organic semiconductors and colloidal quantum dots are attractive candidates for high efficiency, low-cost solar energy harvesting devices. Understanding and controlling the self-assembly of the resulting organic-inorganic nanocomposite films is crucial in optimising device performance, not only at a lab-scale but for large-scale, high-throughput printing and coating methods. Here, grazing incidence X-ray scattering (GIXS) gives direct insights into how small-molecule organic semiconductors and colloidal quantum dots self-assemble during blade coating.

Understanding the Chemical Mechanism behind Photoinduced Enhanced Raman Spectroscopy.

Photoinduced enhanced Raman spectroscopy (PIERS) is a new surface enhanced Raman spectroscopy (SERS) modality with a 680% Raman signal enhancement of adsorbed analytes over that of SERS. Despite the explosion in recent demonstrations, the PIERS mechanism remains undetermined. Using X-ray and time-resolved optical spectroscopies, electron microscopy, cyclic voltammetry, and density functional theory simulations, we elucidate the atomic-scale mechanism behind PIERS.

Mixed Small-Molecule Matrices Improve Nanoparticle Dispersibility in Organic Semiconductor-Nanoparticle Films.

Controlling the dispersibility of nanocrystalline inorganic quantum dots (QDs) within organic semiconductor (OSC):QD nanocomposite films is critical for a wide range of optoelectronic devices. This work demonstrates how small changes to the OSC host molecule can have a dramatic detrimental effect on QD dispersibility within the host organic semiconductor matrix as quantified by grazing incidence X-ray scattering. It is commonplace to modify QD surface chemistry to enhance QD dispersibility within an OSC host.

Bright and stable perovskite light-emitting diodes in the near-infrared range.

Perovskite light-emitting diodes (LEDs) have attracted broad attention due to their rapidly increasing external quantum efficiencies (EQEs). However, most high EQEs of perovskite LEDs are reported at low current densities (<1 mA cm) and low brightness. Decrease in efficiency and rapid degradation at high brightness inhibit their practical applications.