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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Transient Photoresponse of the Tris(2,2'-bipyridine)ruthenium(II)-Catalyzed Minimal 0mate Oscillator
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Transient Photoresponse of the Tris(2,2'-bipyridine)ruthenium(II)-Catalyzed Minimal 0mate Oscillator

机译：Tris（2,2'-联吡啶）钌（II）催化的最小0mate振荡器的瞬态光响应

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摘要

The tris(2,2'-bipyridine)ruthenium(II)-catalyzed minimal bromate oscillator under flow conditions was found to exhibit various dynamical responses to the pulsed-light perturbation in the visible region. The system in its reduced steady state exhibits excitability with a threshold in the applied light-pulse energy, while the oxidized steady state does not respond to the light pulse. The latter exhibits, however, a slow response without a threshold to the negative light pulse. The system in its oscillatory state exhibits a phase shift of oscillations upon application of a pulsed-light perturbation. The oscillation phase is mostly advanced or unaffected, depending on the phase of application of the light pulse, although a narrow region of phase delay has also been found in between. A phase portrait spanned by the redox potential and the bromide ion-selective electrode potential has been determined experimentally on the basis of which the system dynamics is discussed in detail. All these results suggest the importance of the photoproduction of extra HBrO↓(2) upon pulsed-light illumination to induce the autocatalytic process that forces the system to experience a single turn along the limit cycle. A numerical calculation based on the Noyes-Field-Thompson model has supported the proposed features, demonstrating that the pulsed addition of HBrO↓(2) reduces the concentration of Br-quickly. When it is reduced below a certain threshold value, the autocatalytic growth of HBrO↓(2), as well as of the catalyst in its oxidized form, is initiated to exhibit the response corresponding to the observation.
机译：发现在流动条件下，三（2,2'-联吡啶）钌（II）催化的最小溴酸盐振荡器表现出对可见光区域中脉冲光扰动的各种动力学响应。处于降低的稳态的系统在施加的光脉冲能量中具有阈值，而具有激发性，而氧化的稳态对光脉冲没有响应。然而，后者表现出较慢的响应，而对负光脉冲没有阈值。处于振荡状态的系统在施加脉冲光扰动后表现出振荡的相移。取决于光脉冲的施加相位，振荡相位大多提前或不受影响，尽管在它们之间也发现了狭窄的相位延迟区域。已经通过实验确定了由氧化还原电势和溴离子选择电极电势跨越的相像，并在此基础上详细讨论了系统动力学。所有这些结果表明，在脉冲光照射下产生额外的HBrO↓（2）以诱导自动催化过程（迫使系统沿极限循环经历一圈）的光生化的重要性。基于Noyes-Field-Thompson模型的数值计算已经支持了所提出的功能，证明了脉冲添加HBrO↓（2）会迅速降低Br的浓度。当将其降低到某个阈值以下时，HBrO↓（2）以及其氧化形式的催化剂的自催化生长就会启动，以展现与观察结果相对应的响应。

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