Triplet–triplet annihilation photon upconversion (TTA-UC) is a process in which triplet excitons combine to form emissive singlets and holds great promise in biological applications and for improving the spectral match in solar energy conversion. While high TTA-UC quantum yields have been reported for, for example, red-to-green TTA-UC systems, there are only a few examples of visible-to-ultraviolet (UV) transformations in which the quantum yield reaches 10%. In this study, we investigate the performance of six annihilators when paired with the sensitizer 2,3,5,6-tetra(9 H -carbazol-9-yl)benzonitrile (4CzBN), a purely organic compound that exhibits thermally activated delayed fluorescence. We report a record-setting internal TTA-UC quantum yield (Φ UC,g ) of 16.8% (out of a 50% maximum) for 1,4-bis((triisopropylsilyl)ethynyl)naphthalene, demonstrating the first example of a visible-to-UV TTA-UC system approaching the classical spin-statistical limit of 20%. Three other annihilators, of which 2,5-diphenylfuran has never been used for TTA-UC previously, also showed impressive performances with Φ UC,g above 12%. In addition, a new method to determine the rate constant of TTA is proposed, in which only time-resolved emission measurements are needed, circumventing the need for more challenging transient absorption measurements. The results reported herein represent an important step toward highly efficient visible-to-UV TTA-UC systems that hold great potential for driving high-energy photochemical reactions.

Novel approaches to modify the spectral output of the sun have seen a surge in interest recently, with triplet–triplet annihilation driven photon upconversion (TTA-UC) gaining widespread recognition due to its ability to function under low-intensity, noncoherent light. Herein, four diphenylanthracene (DPA) dimers are investigated to explore how the structure of these dimers affects upconversion efficiency. Also, the mechanism responsible for intramolecular upconversion is elucidated. In particular, two models are compared using steady-state and time-resolved simulations of the TTA-UC emission intensities and kinetics. All dimers perform TTA-UC efficiently in the presence of the sensitizer platinum octaethylporphyrin. The meta-coupled dimer 1,3-DPA 2 performs best yielding a 21.2% upconversion quantum yield (out of a 50% maximum), which is close to that of the reference monomer DPA (24.0%). Its superior performance compared to the other dimers is primarily ascribed to the longer triplet lifetime of this dimer (4.7 ms), thus reinforcing the importance of this parameter. Comparisons between simulations and experiments reveal that the double-sensitization mechanism is part of the mechanism of intramolecular upconversion and that this additional pathway could be of great significance under specific conditions. The results from this study can thus act as a guide not only in terms of annihilator design but also for the design of future solid-state systems where intramolecular exciton migration is anticipated to play a major role.

Developing high-performance visible-to-UV photon upconversion systems based on triplet-triplet annihilation photon upconversion (TTA-UC) is highly desired, as it provides a potential approach for UV light-induced photosynthesis and photocatalysis. However, the quantum yield and spectral range of visible-to-UV TTA-UC based on nanocrystals (NCs) are still far from satisfactory. Here, three different sized CdS NCs are systematically investigated with triplet energy transfer to four mediators and four annihilators, thus substantially expanding the available materials for visibleto-UV TTA-UC. By improving the quality of CdS NCs, introducing the mediator via a direct mixing fashion, and matching the energy levels, a high TTA-UC quantum yield of 10.4% (out of a 50% maximum) is achieved in one case, which represents a record performance in TTA-UC based on NCs without doping. In another case, TTA-UC photons approaching 4 eV are observed, which is on par with the highest energies observed in optimized organic systems. Importantly, the in-depth investigation reveals that the direct mixing approach to introduce the mediator is a key factor that leads to close to unity efficiencies of triplet energy transfer, which ultimately governs the performance of NC-based TTA-UC systems. These findings provide guidelines for the design of high-performance TTA-UC systems toward solar energy harvesting.

Triplet–triplet annihilation photon upconversion (TTA-UC) is a process in which low-energy light is transformed into light of higher energy. During the last two decades, it has gained increasing attention due to its potential in, e.g., biological applications and solar energy conversion. The highest efficiencies for TTA-UC systems have been achieved in liquid solution, owing to that several of the intermediate steps require close contact between the interacting species, something that is more easily achieved in diffusion-controlled environments. There is a good understanding of the kinetics dictating the performance in liquid TTA-UC systems, but so far, the community lacks cohesiveness in terms of how several important parameters are best determined experimentally. In this perspective, we discuss and present a “best practice” for the determination of several critical parameters in TTA-UC, namely triplet excited state energies, rate constants for triplet–triplet annihilation ($$k_{{{\text{TTA}}}}$$ k TTA ), triplet excited-state lifetimes ($$\tau_{{\text{T}}}$$ τ T ), and excitation threshold intensity ($$I_{{{\text{th}}}}$$ I th ). Finally, we introduce a newly developed method by which $$k_{{{\text{TTA}}}}$$ k TTA , $$\tau_{{\text{T}}}$$ τ T , and $$I_{{{\text{th}}}}$$ I th may be determined simultaneously using the same set of time-resolved emission measurements. The experiment can be performed with a simple experimental setup, be ran under mild excitation conditions, and entirely circumvents the need for more challenging nanosecond transient absorption measurements, a technique that previously has been required to extract $$k_{{{\text{TTA}}}}$$ k TTA . Our hope is that the discussions and methodologies presented herein will aid the photon upconversion community in performing more efficient and manageable experiments while maintaining—and sometimes increasing—the accuracy and validity of the extracted parameters.

We need clean drinking water, but current water purification methods are not always sufficient. This study examines the binding and binding mechanisms when graphene oxide is used as a filter material for removing perfluorinated substances and trihalomethanes. We use density functional theory calculations to examine the binding of the harmful molecules on graphene oxide. Our results indicate that the binding energies between graphene oxide and the investigated molecules are in the range of 370–1450 meV per molecule, similar to the binding energies obtained in other studies, where adsorption of similar size molecules onto graphene oxide has been investigated. This indicates that graphene oxide has the potential to separate the molecules of interest from the water. Significant contribution to the binding energies comes from the van der Waals (dispersion) interaction between the molecule and graphene oxide, while the hydrogen bonding between the functional groups of graphene oxide and the hydrogen atoms in functional groups on the molecules also plays a role in the binding.