Nonradiative relaxation processes in condensed phases.

机译：凝聚相的非辐射弛豫过程。

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In this thesis we consider two particular cases of nonradiative decay: multiphonon relaxation in solids and vibrational energy relaxation in liquids. In Chapter 2, we develop a microscopic theory of multiphonon relaxation. Two alternative mechanisms of the relaxation process are presented and their relative importance is discussed. For each approach a closed-form analytical expression for the relaxation rate is given as a function of energy gap and temperature. In Chapter 3, we apply our theory to analyze the energy gap- and temperature-dependent experimental data for various electronic transitions of rare-earth impurities in YAlO{dollar}sb3{dollar} host. In Chapter 4, we focus on the vibrational energy relaxation of diatomics in rare gas crystals. The predictions of the theory are compared with the experimental data on the relaxation of O{dollar}sb2{dollar} in solid Ar. In Chapter 5, we develop a microscopic theory of the vibrational energy relaxation of a diatomic solute in an atomic solvent. Our treatment is based on the force-force time-correlation function approach, and involves a short-time expansion of the correlation function. Theoretical results for the relaxation rate are compared to experiments on I{dollar}sb2{dollar} in Xe over a wide range of densities and temperatures.

机译：在本文中，我们考虑了两种非辐射衰减的特殊情况：固体中的多声子弛豫和液体中的振动能弛豫。在第二章中，我们发展了多声子弛豫的微观理论。介绍了松弛过程的两种替代机制，并讨论了它们的相对重要性。对于每种方法，均给出了弛豫率的封闭形式分析表达式，其为能隙和温度的函数。在第3章中，我们应用我们的理论分析了YAlO {sal} sb3 {dollar}主体中稀土杂质各种电子跃迁的能隙和温度相关实验数据。在第4章中，我们重点讨论稀有气体晶体中双原子的振动能量弛豫。将该理论的预测结果与O {dollar} sb2 {dollar}在固态Ar中弛豫的实验数据进行了比较。在第5章中，我们发展了原子溶剂中双原子溶质的振动能弛豫的微观理论。我们的处理基于力-时间相关函数方法，并且涉及相关函数的短时扩展。将弛豫率的理论结果与Xe上I {dollar} sb2 {dollar}在较大密度和温度范围内的实验进行了比较。

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作者
Egorov, Sergey Alexeevich.;
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作者单位

The University of Wisconsin - Madison.;

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授予单位 The University of Wisconsin - Madison.;
学科 Chemistry Physical.
学位 Ph.D.
年度 1996
页码 165 p.
总页数 165
原文格式 PDF
正文语种 eng
中图分类物理化学（理论化学）、化学物理学;
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1. Nonradiative relaxation processes in condensed phases: Quantum versus classical baths [J] . S. A. Egorov, Eran Rabani, B. J. Berne The Journal of Chemical Physics . 1999,第11期

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Nonradiative relaxation processes in condensed phases.

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