Almazova Natalya, Aubry Serge, Tsironis Giorgos P
Institute of Theoretical and Computational Physics, Department of Physics, University of Crete, 71003 Heraklion, Greece.
Entropy (Basel). 2024 Sep 2;26(9):753. doi: 10.3390/e26090753.
Ultrafast reaction processes take place when resonant features of nonlinear model systems are taken into account. In the targeted energy or electron transfer dimer model this is accomplished through the implementation of nonlinear oscillators with opposing types of nonlinearities, one attractive while the second repulsive. In the present work, we show that this resonant behavior survives if we take into account the vibrational degrees of freedom as well. After giving a summary of the basic formalism of chemical reactions we show that resonant electron transfer can be assisted by vibrations. We find the condition for this efficient transfer and show that in the case of additional interaction with noise, a distinct non-Arrhenius behavior develops that is markedly different from the usual Kramers-like activated transfer.
当考虑非线性模型系统的共振特性时，超快反应过程就会发生。在目标能量或电子转移二聚体模型中，这是通过实现具有相反类型非线性的非线性振荡器来完成的，一种是吸引性的，另一种是排斥性的。在本工作中，我们表明，如果我们也考虑振动自由度，这种共振行为仍然存在。在给出化学反应基本形式的总结之后，我们表明共振电子转移可以由振动辅助。我们找到了这种有效转移的条件，并表明在与噪声有额外相互作用的情况下，会出现一种明显的非阿仑尼乌斯行为，它与通常的类似克莱默斯的活化转移明显不同。
