Molecular Systems Design & Engineering, Journal Year: 2024, Volume and Issue: 9(4), P. 423 - 435
Published: Jan. 1, 2024
A systematic search for novel singlet fission materials based on the recently synthesized 6,6′-biphenanthridine (biphe) framework is reported, utilizing a straightforward computational approach.
Language: Английский
Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 1, 2025
The emerging field of quantum life science combines principles from physics and biology to study fundamental processes at the molecular level.
Language: Английский
Citations
3
Science Advances, Journal Year: 2024, Volume and Issue: 10(1)
Published: Jan. 3, 2024
Singlet fission can generate an exchange-coupled quintet triplet pair state
Citations
13
Small, Journal Year: 2024, Volume and Issue: 20(34)
Published: April 8, 2024
Oxygen evolution reaction (OER) is a widely employed half-electrode in oxygen electrochemistry, applications such as hydrogen evolution, carbon dioxide reduction, ammonia synthesis, and electrocatalytic hydrogenation. Unfortunately, its slow kinetics limits the commercialization of applications. It therefore highly imperative to develop robust electrocatalysts with high activity, long-term durability, low noble-metal contents. Previously intensive efforts have been made introduce advancements on developing non-precious transition metal their OER mechanisms. Electronic structure tuning one most effective interesting ways boost activity spin angular momentum an intrinsic property electron. Therefore, modulation states magnetic properties electrocatalyst enables changes energy associated interacting electron clouds radical absorbance, affecting stability. Given that few review this topic, review, the-state-of-the-art research progress spin-dependent effects will be briefed. Spin engineering strategies, strain, crystal surface engineering, doping, etc., introduced. The related mechanism for manipulation also discussed. Finally, challenges prospects development catalysis are presented. This aims highlight significance breaking bottleneck electrocatalysis promoting practical application high-efficiency electrocatalysts.
Language: Английский
Citations
10
Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(38), P. 20883 - 20896
Published: Sept. 14, 2023
Covalent dimers, particularly pentacenes, are the dominant platform for developing a mechanistic understanding of intramolecular singlet fission (iSF). Numerous studies have demonstrated that photoexcited state in these structures can rapidly and efficiently undergo exciton multiplication to form correlated pair triplets within single molecule, with potential applications from photovoltaics quantum information science. One most significant barriers limiting such dimers is fast recombination triplet pair, which prevents spatial separation formation long-lived states. There an ever-growing need develop general synthetic strategies control evolution following iSF enhance their lifetime. Here, we rationally tune dihedral angle interchromophore between pairs pentacenes systematic series bridging units facilitate separation. Through combination transient optical spin-resonance techniques, demonstrate torsion linker provides simple handle fine balance through-bond through-space couplings steer iSF. We show full pathway femtosecond microsecond timescales tuned through static coupling set by molecular design structural fluctuations be biased steric control. Our approach highlights straightforward principle generate paramagnetic spin states higher yields.
Language: Английский
Citations
24
Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(28), P. 15275 - 15283
Published: July 7, 2023
The quintet triplet-pair state may be generated upon singlet fission and is a critical intermediate that dictates the fate of excitons, which can exploited for photovoltaics, information technologies, biomedical imaging. In this report, we demonstrate continuous-wave pulsed electron spin resonance techniques such as phase-inverted echo-amplitude detected nutation (PEANUT), have emerged primary tool identifying pathways in fission, probe fundamentally different species. We directly observe generation rate high-spin triplet pairs dependent on molecular orientation with respect to static magnetic field. Moreover, observation prevent incorrect analysis (cw-ESR) measurements provide insight into design materials target specific optimize exciton properties applications.
Language: Английский
Citations
16
Communications Physics, Journal Year: 2023, Volume and Issue: 6(1)
Published: April 8, 2023
Abstract Singlet fission describes the spin-conserving production of two triplet excitons from one singlet exciton. The existence a spin-2 (quintet) triplet-pair state as product is well established in literature, and control quintet formation an important step towards applying photovoltaics quantum information. However, definitive mechanism for yet to be established, which makes it difficult design materials optimal formation. Here we outline inter-triplet exchange-coupling fluctuations drive fast efficient We show that possible even strong-exchange regime, accordance with recent experimental prediction. evaluate performance this regimes conformational freedom, relate dynamics material properties molecules.
Language: Английский
Citations
15
The Journal of Physical Chemistry Letters, Journal Year: 2023, Volume and Issue: 14(27), P. 6241 - 6247
Published: July 4, 2023
Solution-state nuclear magnetic resonance spectroscopy (NMR) is a powerful method for the analysis of intermolecular interactions within biomolecular system. However, low sensitivity one major obstacles NMR. We improved solution-state 13C NMR observation between protein and ligand using hyperpolarized solution samples at room temperature. Eutectic crystals composed 13C-salicylic acid benzoic doped with pentacene were by dynamic polarization photoexcited triplet electrons, 0.72 ± 0.07% was achieved after dissolution. The binding human serum albumin 13C-salicylate observed several hundred times enhancement under mild conditions. established applied pharmaceutical experiments partial return chemical shift salicylate competitive other non-isotope-labeled drugs.
Language: Английский
Citations
14
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(8)
Published: Jan. 5, 2024
Abstract A series of ferrocene(Fc)‐bridged pentacene(Pc)‐dimers [Fc−Ph(2, n )−(Pc) 2 : =number phenylene spacers] were synthesized to examine the tortional motion effect Fc‐terminated linkers on strongly coupled quintet multiexciton ( 5 TT) formation through intramolecular singlet fission (ISF). Fc−Ph(2,4)−(Pc) has a relatively small electronic coupling and large conformational flexibility according spectroscopic theoretical analyses. exhibits high‐yield TT together with quantitative 1 generation ISF. This demonstrates much more efficient ISF than those other less flexible Pc dimers. The activation entropy in spin conversion is larger systems due associated torsional linkers. attributable weakened metal‐ligand bonding Fc hybridization hole level unpaired orbitals.
Language: Английский
Citations
6
Progress in Nuclear Magnetic Resonance Spectroscopy, Journal Year: 2024, Volume and Issue: 142-143, P. 55 - 68
Published: May 16, 2024
Dynamic nuclear polarization (DNP) is a method for achieving high levels of spin by transferring from electrons to nuclei microwave irradiation, resulting in higher sensitivity NMR/MRI. In particular, DNP using photoexcited triplet electron spins (triplet-DNP) can provide hyperpolarized state at room temperature and low magnetic field. this review article, we highlight recent developments materials instrumentation the application triplet-DNP. First, brief history principles triplet-DNP will be presented. Next, important advances years outlined: new hyperpolarize water biomolecules; high-sensitivity solution NMR dissolution triplet-DNP; strategies further improvement polarization. view these developments, future directions widen range applications discussed.
Language: Английский
Citations
5
Chemical Science, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 4, 2024
Anion recognition in water by synthetic host molecules is a popular and challenging topic. It has been considered difficult because the compete for units. In this study, we have successfully created novel macrocycle that achieves precise through multipoint hydrogen bonding harmony with molecules. Specifically, an
Language: Английский
Citations
4