A new approach to radiationless decay phenomena by generalization of the Mori theory

P. Grigolini , V. Rosato
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引用次数: 2

Abstract

A suitable extension of the Mori theory to deal with non-hermitian hamiltonians leads to a rigorous justification of models of “reduced” kind for radiationless decay phenomena. By using the model of an excited state sequentially coupled to two dissipative quasicontinua it is shown that the generalized theory leads to a reduced model consisting of only two “virtual” states. The standard Mori approach, on the contrary, would result in a chain of more than two states (probably an infinite number of states). It is shown, furthermore, that the biexponential decay behaviour can rigorously be justified in two different ways. The first model only consisists ofcouplings of intramolecular type. The second model also involves an external thermal bath. The generalized Mori theory, when applied to the second model leads to a non phenomenological justification for the kinetic scheme. It is shown, furthermore, that excitations by strong radiation fields result in a different decay behaviour according to whether the former or the latter scheme is applied.

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推广Mori理论研究无辐射衰变现象的新方法
对莫里理论进行适当的扩展,以处理非厄米哈密顿量,从而对无辐射衰变现象的“简化”类模型进行了严格的证明。利用一个激发态序列耦合到两个耗散拟连续态的模型,证明了广义理论可以得到一个仅由两个“虚”态组成的简化模型。与此相反,标准的Mori方法将产生一个由两个以上状态(可能是无限多个状态)组成的链。进一步表明,双指数衰减行为可以用两种不同的方式严格地证明。第一种模式只包括分子内型的偶联。第二种模式也包括外部热浴。当将广义Mori理论应用于第二个模型时,会导致动力学方案的非现象学正当性。此外,强辐射场的激发会导致不同的衰变行为,这取决于采用前一种方案还是后一种方案。
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