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Singlet fission in organic semiconductors causes a singlet exciton to decay into a pair of triplet excitons and holds potential for increasing the efficiency of photovoltaic devices. In this combined experimental and theoretical study, we reveal that a covalent dimer of the organic semiconductor tetracene undergoes activated singlet fission by qualitatively different mechanisms depending on the solvent environment. We show that intramolecular vibrations are an integral part of this mechanism, giving rise to mixing between charge transfer and triplet pair excitations. Both coherent or incoherent singlet fission can occur, depending on transient solvent-induced energetic proximity between the states, giving rise to complex variation of the singlet fission mechanism and timescale in the different environments. Our results suggest a more general principle for controlling the efficiency of photochemical reactions by utilizing transient interactions to tune the energetics of reactant and product states and switch between incoherent and coherent dynamics.
This article was published in the following journal.
Name: Journal of the American Chemical Society
Singlet fission of carotenoid excitation is studied in purple phototrophic bacterium Thermochromatium tepidum. Using time-resolved EPR and magnetic field-induced modulation of fluorescence yield it is...
Intramolecular singlet fission and triplet-triplet annihilation (TTA) has been experimentally observed and reported. However, problems remain in theoretically accounting for the corresponding intramol...
Singlet fission directly from upper excited vibrational and electronic states of cofacial perylene dimers bypassing the relaxed state S1 was detected within 50 fs. This process competes well with vibr...
Singlet fission is known to improve solar energy utilization by circumventing the Shockley-Queisser limit. The two essential steps of singlet fission are the formation of a correlated triplet pair and...
Tetracene is the archetypal material undergoing singlet fission - the generation of a pair of triplet excitons from one singlet exciton. Here, using time-resolved electron spin resonance, we show how ...
A non-fission sourced, solvent generator produced 99mTc intravenous injection, as 99mTc -MDP, is to be used as a bone scan diagnostic radiopharmaceutical for assessment of bone pathology u...
No clinical evidence has been yet published regarding the comparison of postoperative pain after removal of the root canal fillings with or without solvent. The aim of this study was to ev...
Our preliminary data suggests that pharmacological inhibition of the mitochondrial fission protein, Drp1, reduced atherosclerotic plaque volume and attenuated macrophage accumulation withi...
The purpose of the study is to monitor the safety of FS VH S/D and evaluate whether FS VH S/D is superior to standard treatment in reducing blood loss in subjects undergoing total hip repl...
Hyperprolactinaemia is a common side effect of some antipsychotics (APS), including some atypicals. Clinical consequences of hyperprolactinaemia are broad including amenorrhea, galactorrhe...
An excited state of molecular oxygen generated photochemically or chemically. Singlet oxygen reacts with a variety of biological molecules such as NUCLEIC ACIDS; PROTEINS; and LIPIDS; causing oxidative damages.
Gene rearrangement of the B-lymphocyte which results in a substitution in the type of heavy-chain constant region that is expressed. This allows the effector response to change while the antigen binding specificity (variable region) remains the same. The majority of class switching occurs by a DNA recombination event but it also can take place at the level of RNA processing.
The pressure required to prevent the passage of solvent through a semipermeable membrane that separates a pure solvent from a solution of the solvent and solute or that separates different concentrations of a solution. It is proportional to the osmolality of the solution.
Devices containing fissionable material in sufficient quantity and so arranged as to be capable of maintaining a controlled, self-sustaining NUCLEAR FISSION chain reaction. They are also known as atomic piles, atomic reactors, fission reactors, and nuclear piles, although such names are deprecated. (McGraw-Hill Dictionary of Scientific and Technical Terms, 4th ed)
Abnormally high temperature intentionally induced in living things regionally or whole body. It is most often induced by radiation (heat waves, infra-red), ultrasound, or drugs.