The few known reports and the likely prospects of finding new efficient routes to exciton fission from higher excited singlet states, S ( > 1), are reviewed. Aggregates of molecules that have large S-S electronic energy spacings and/or emit measurable "contra-Kasha" emission may offer further opportunities. Among these, electronically excited molecular systems that exhibit known efficient (T + T) triplet-triplet annihilation producing S could exhibit efficient singlet fission in aggregates when appropriately substituted to meet the necessary energy requirements. The potential problem of loss of triplet excitons 2T → T + S triplet-triplet annihilation following (S + S) singlet fission is addressed. Aggregates of substituted azulenes and aliphatic thiones and dithiones are particularly attractive and are discussed in detail.
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http://dx.doi.org/10.1039/d3cp03201a | DOI Listing |
J Am Chem Soc
January 2025
Radiation Laboratory, University of Notre Dame, Notre Dame, Indiana 46556, United States.
Modulation of singlet and triplet energy transfer from excited semiconductor nanocrystals to attached dye molecules remains an important criterion for the design of light-harvesting assemblies. Whereas one can consider the selection of donor and acceptor with favorable energetics, spectral overlap, and kinetics of energy transfer as a means to direct the singlet and triplet energy transfer pathways, it is not obvious how to control the singlet and triplet characteristics of the donor semiconductor nanocrystal itself. By doping CsPb(ClBr) nanocrystals with Mn, we have now succeeded in increasing the triplet characteristics of semiconductor nanocrystals.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
Mulliken Center for Theoretical Chemistry, Clausius Institute for Physical and Theoretical Chemistry, Rheinische Friedrich-Wilhelms Universität Bonn, Beringstraße 4, 53115 Bonn, Germany.
With their narrow-band emission, high quantum yield, and good chemical stability, multiresonance thermally activated delayed fluorescence (MR-TADF) emitters are promising materials for OLED technology. However, accurately modeling key properties, such as the singlet-triplet (ST) energy gap and fluorescence energy, remains challenging. While time-dependent density functional theory (TD-DFT), the workhorse of computational materials science, suffers from fundamental issues, wave function-based coupled-cluster (CC) approaches, like approximate CC of second-order (CC2), are accurate but suffer from high computational cost and unfavorable scaling with system size.
View Article and Find Full Text PDFSmall
January 2025
Department of Botany and Microbiology, College of Science, King Saud University, P.O. Box 2455, Riyadh, 11451, Saudi Arabia.
A polyacrylamide gel method has been used to synthesize a variety of polyvalent-transition-metal-doped Ni position of high entropy spinel oxides (NiZnMgCuCo)AlO-800 °C (A) on the basis of NiAlO, and the catalytic activity of A is studied under the synergistic action of peroxymonosulfate (PMS) activation and simulated sunlight. The A containing polyvalent transition metals (Ni, Cu, and Co) can effectively activate PMS and efficiently degrade levofloxacin (LEV) and tetracycline hydrochloride (TCH) under simulated sunlight irradiation. After 90 min of light exposure, the degradation percentages of LEV (50 mg L) and TCH (100 mg L) degrade by the A/PMS/vis system reach 87.
View Article and Find Full Text PDFJ Phys Chem Lett
January 2025
Department of Chemical Engineering, School of Chemistry and Chemical Engineering, Nanchang University, Nanchang 330031, China.
Lithium-sulfur batteries have been recognized as one of the excellent candidates for next-generation energy storage batteries because of their high energy density and low cost and low pollution. However, lithium-sulfur batteries have been challenged by low conductivity, low sulfur utilization, poor cycle life, and the shuttle effect of polysulfides. To address these problems, we report here an independent mixed sulfur host.
View Article and Find Full Text PDFSci Rep
January 2025
School of Physics, Sun Yat-Sen University, Guangzhou, 510275, People's Republic of China.
The ground states of two-species condensates with spin-1 atoms have been studied analytically and numerically. All the results from the analytical approach are checked by the latter. The [Formula: see text] channel has been neglected, where λ is the coupled spin of two different atoms.
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