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1.
J Am Chem Soc ; 146(18): 12324-12328, 2024 May 08.
Artigo em Inglês | MEDLINE | ID: mdl-38661382

RESUMO

This study reports a comparison of the kinetics of electrochemical (EC) versus photoelectrochemical (PEC) water oxidation on bismuth vanadate (BiVO4) photoanodes. Plots of current density versus surface hole density, determined from operando optical absorption analyses under EC and PEC conditions, are found to be indistinguishable. We thus conclude that EC water oxidation is driven by the Zener effect tunneling electrons from the valence to conduction band under strong bias, with the kinetics of both EC and PEC water oxidation being determined by the density of accumulated surface valence band holes. We further demonstrate that our combined optical absorption/current density analyses enable an operando quantification of the BiVO4 photovoltage as a function of light intensity.

2.
J Am Chem Soc ; 146(19): 13133-13141, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38695282

RESUMO

Triphenylmethyl (trityl) radicals have shown potential for use in organic optoelectronic applications, but the design of practical trityl structures has been limited to donor/radical charge-transfer systems due to the poor luminescence of alternant symmetry hydrocarbons. Here, we circumvent the symmetry-forbidden transition of alternant hydrocarbons via excited-state symmetry breaking in a series of phenyl-substituted tris(2,4,6-trichlorophenyl)methyl (TTM) radicals. We show that 3-fold phenyl substitution enhances the emission of the TTM radical and that steric control modulates the optical properties in these systems. Simple ortho-methylphenyl substitution boosts the photoluminescence quantum efficiency from 1% (for TTM) to 65% at a peak wavelength of 612 nm (for 2-T3TTM) in solution. In the crystalline solid state, the neat 2-T3TTM radical shows a remarkably high photoluminescence quantum efficiency of 25% for emission peaking at 706 nm. This has implications in the design of aryl-substituted radical structures where the electronic coupling of the substituents influences variables such as emission, charge transfer, and spin interaction.

3.
Inorg Chem ; 59(12): 8127-8133, 2020 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-32484663

RESUMO

The magnetic properties of the spin-5/2 double molybdate LiFe(MoO4)2 have been characterized by heat capacity, magnetic susceptibility, and neutron powder diffraction techniques. Unlike the multiferroic system LiFe(WO4)2 which exhibits two successive magnetic transitions, LiFe(MoO4)2 undergoes only one antiferromagnetic transition at TN ∼ 23.8 K. Its antiferromagnetic magnetic structure with the commensurate propagation vector k = (0, 0.5, 0) has been determined. Density functional theory calculations confirm the antiferromagnetic ground state and provide a numerical estimate of the relevant exchange coupling constants.

4.
Math Biosci Eng ; 21(3): 4501-4520, 2024 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-38549338

RESUMO

We investigated synchronization of dynamic systems with mixed delays and delayed impulses. Using impulsive control method and the average impulsive interval approach, several Lyapunov sufficient conditions were given for ensuring synchronization in terms of impulsive perturbation and impulsive control, respectively. The derived conditions indicated that delays in continuous dynamical systems were flexible under impulsive perturbation and were not strictly dependent on the size of impulsive delays, and they may have a potential impact on synchronization of the considered system. In addition, applying the proposed concepts of average positive impulsive estimation and average impulsive estimation, we integrated the information in impulsive delay into the rate coefficient to eliminate the limitation of having the same threshold at each impulse point, while the impulsive delay maintained the synchronization effect. This was an improvement on the previous results obtained. Finally, we provided two numerical examples to illustrate the validity of our results.

5.
Artigo em Inglês | MEDLINE | ID: mdl-38709607

RESUMO

Activation functions have a significant effect on the dynamics of neural networks (NNs). This study proposes new nonmonotonic wave-type activation functions and examines the complete stability of delayed recurrent NNs (DRNNs) with these activation functions. Using the geometrical properties of the wave-type activation function and subsequent iteration scheme, sufficient conditions are provided to ensure that a DRNN with n neurons has exactly (2m + 3)n equilibria, where (m + 2)n equilibria are locally exponentially stable, the remainder (2m + 3)n - (m + 2)n equilibria are unstable, and a positive integer m is related to wave-type activation functions. Furthermore, the DRNN with the proposed activation function is completely stable. Compared with the previous literature, the total number of equilibria and the stable equilibria significantly increase, thereby enhancing the memory storage capacity of DRNN. Finally, several examples are presented to demonstrate our proposed results.

6.
Math Biosci Eng ; 20(8): 14846-14865, 2023 Jul 10.
Artigo em Inglês | MEDLINE | ID: mdl-37679162

RESUMO

In this paper, the complete synchronization and Mittag-Leffler synchronization problems of a kind of coupled fractional-order neural networks with time-varying delays are introduced and studied. First, the sufficient conditions for a controlled system to reach complete synchronization are established by using the Kronecker product technique and Lyapunov direct method under pinning control. Here the pinning controller only needs to control part of the nodes, which can save more resources. To make the system achieve complete synchronization, only the error system is stable. Next, a new adaptive feedback controller is designed, which combines the Razumikhin-type method and Mittag-Leffler stability theory to make the controlled system realize Mittag-Leffler synchronization. The controller has time delays, and the calculation can be simplified by constructing an appropriate auxiliary function. Finally, two numerical examples are given. The simulation process shows that the conditions of the main theorems are not difficult to obtain, and the simulation results confirm the feasibility of the theorems.

7.
IEEE Trans Neural Netw Learn Syst ; 34(12): 10970-10979, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-35552146

RESUMO

Interval bipartite consensus of multiagents described by signed graphs has received extensive concern recently, and the rooted cycles play a critical role in stabilization, while the structurally balanced graphs are essential to achieve bipartite consensus. However, the gauge transformation used in the linear system is no longer feasible in the nonlinear case. This article addresses interval bipartite synchronization of multiple neural networks (NNs) in a signed graph via a Lyapunov-based approach, extending the existing work to a more practical but complicated case. A general matrix M in signed graphs is introduced to construct the novel Lyapunov functions, and sufficient conditions are obtained. We find that the rooted cycles and the structurally balanced graphs are essential to stabilize and achieve bipartite synchronization. More importantly, we discover that the nonrooted cycles are crucial in reaching interval bipartite synchronization, not previously mentioned. Several examples are presented to illustrate interval bipartite synchronization of multiple NNs with signed graphs.

8.
IEEE Trans Cybern ; 53(10): 6277-6288, 2023 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-35439156

RESUMO

The time-triggered impulsive controls were widely used to study the collective behavior of homogeneous dynamical networks due to their low control cost, which was a bit conservative in the occupation of communication channels. This article addresses designing the event-triggered impulsive controls for the quasisynchronization, namely, a weak cooperative behavior with the synchronization error no more than a positive constant in the leader-following heterogeneous dynamical network, which thus can reduce the occupation of resources significantly. The centralized and distributed impulsive controls are designed to lead the followers to synchronize approximately to the leader within a nonzero bound, where the impulsive instants are triggered, respectively, by the global or local state-dependent conditions. Numerical results are put forward to verify the effectiveness of the proposed methods.

9.
Nat Commun ; 14(1): 4147, 2023 Jul 12.
Artigo em Inglês | MEDLINE | ID: mdl-37438369

RESUMO

Neutral π-radicals have potential for use as light emitters in optoelectronic devices due to the absence of energetically low-lying non-emissive states. Here, we report a defect-free synthetic methodology via mesityl substitution at the para-positions of tris(2,4,6-trichlorophenyl)methyl radical. These materials reveal a number of novel optoelectronic properties. Firstly, mesityl substituted radicals show strongly enhanced photoluminescence arising from symmetry breaking in the excited state. Secondly, photoexcitation of thin films of 8 wt% radical in 4,4'-bis(carbazol-9-yl)-1,1'-biphenyl host matrix produces long lived (in the order of microseconds) intermolecular charge transfer states, following hole transfer to the host, that can show unexpectedly efficient red-shifted emission. Thirdly, covalent attachment of carbazole into the mesitylated radical gives very high photoluminescence yield of 93% in 4,4'-bis(carbazol-9-yl)-1,1'-biphenyl films and light-emitting diodes with maximum external quantum efficiency of 28% at a wavelength of 689 nm. Fourthly, a main-chain copolymer of the mesitylated radical and 9,9-dioctyl-9H-fluorene shows red-shifted emission beyond 800 nm.

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