Abstract
Before lasers were brought to the laboratories of chemists and physicists, molecular relaxations were identified using broad band chaotic light excitation. Knowledge of the radiative decay from the photon counting rate and the quantum yield gives information about one of the most fundamental processes in chemical dynamics; radiationless transitions. From the last two decades much is known about these processes, which simply result in a change of molecular electronic state without absorption or emission of photons. and encompass a wide class of phenomena such as autoionization in atoms, predissociation, molecular electronic relaxation and energy transport in condensed media. What is not known, at least experimentally, can be outlined with the following questions:
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(1)
Do radiationless transitions depend on the nature of the exciting photon field?
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(2)
What is the exact nature of the state we excite?
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(3)
What is the influence of the ensemble optical coherence on the evolution of nonradiative processes?
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(4)
Is there a threshold for an “ergodic” behavior in large molecules?
Contribution No. 5634.
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References
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For long time pulses, the Fourier transformed width is 10 KHz, which is much less than the (jitter included) effective width of the laser. In the pentacene system, one sees clearly the decay when the long time pulse is on or off. For short pulses, the pulse-on decay is similar to the long pulse case but the pulse-off decay exhibits a fast decay component that we ascribe due to population inversion in the originally pumped group of molecules [9].
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Zewail, A.H. (1977). Coherent Optical Spectroscopy of Molecules Undergoing Resonance Scattering and Radiationless Transitions: The Right-Angle Photon Echo. In: Hall, J.L., Carlsten, J.L. (eds) Laser Spectroscopy III. Springer Series in Optical Sciences, vol 7. Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-540-35968-5_30
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DOI: https://doi.org/10.1007/978-3-540-35968-5_30
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