Equivalence between the mechanical model and energy-transfer theory for the classical decay rates of molecules near a spherical particle

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Original languageEnglish
Article number184106
Journal / PublicationJournal of Chemical Physics
Issue number18
Publication statusPublished - 14 May 2012
Externally publishedYes


In the classical modeling of decay rates for molecules interacting with a nontrivial environment, it is well known that two alternate approaches exist which include: (1) a mechanical model treating the system as a damped harmonic oscillator driven by the reflected fields from the environment; and (2) a model based on the radiative and nonradiative energy transfers from the excited molecular system to the environment. While the exact equivalence of the two methods is not trivial and has been explicitly demonstrated only for planar geometry, it has been widely taken for granted and applied to other geometries such as in the interaction of the molecule with a spherical particle. Here we provide a rigorous proof of such equivalence for the molecule-sphere problem via a direct calculation of the decay rates adopting each of the two different approaches. © 2012 American Institute of Physics.

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