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Laser Excitation of Stationary States in Molecules: The Coupling of Real Eigenstates to Phonons and Photons

Zewail, A. H. and Jones, K. E. and Orlowski, T. E. (1977) Laser Excitation of Stationary States in Molecules: The Coupling of Real Eigenstates to Phonons and Photons. Spectroscopy Letters, 10 (2). pp. 115-125. ISSN 0038-7010. doi:10.1080/00387017708067501.

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When a molecule is excited by a light source one considers the following optical cycle; absorption to a singlet state, internal conversion, intersystem crossing, and finally a phosphorescence from the triplet state (Jablonski process) to the ground state. On the other hand, one knows from quantum mechanics that a singlet state isoenergetic with other singlets or triplets interacts with these levels thus producing new states which diagonalize the exact molecular Hamiltonian. The question of course; which state do we excite and under what conditions does the intermolecular interaction (say with a phonon bath) influence the pathways for the excitation process? In this communication we will present for the first time experimental evidence for the laser excitation of true eigenstates in molecules. We will also discuss the theoretical treatment and the experimental findings on thermal broadening of electronic resonances which result in the loss of the “identity” of molecular states. Finally, it will be shown that vibrational relaxation and magnetic field induced couplings depend crucially on the preparation of the state.

Item Type:Article
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Additional Information:© 1977 Taylor & Francis.
Subject Keywords:Photons, phonons, radiationless transitions, Born-Oppenheimer states, laser spectroscopy,
Issue or Number:2
Record Number:CaltechAUTHORS:20161005-085507124
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:70866
Deposited By: Ruth Sustaita
Deposited On:05 Oct 2016 16:15
Last Modified:11 Nov 2021 04:36

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