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Radiationless decay in exciplexes with variable charge transfer.

Ian R Gould1, Samir Farid

  • 1Department of Chemistry and Biochemistry, Arizona State University, Tempe, Arizona 85287-1604, USA. igould@asu.edu

The Journal of Physical Chemistry. B
|June 15, 2007
PubMed
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This study quantifies decay rates in excited states, revealing how charge transfer extent dictates radiative versus radiationless processes. Understanding these factors is key for controlling excited-state dynamics in photochemistry.

Area of Science:

  • Photochemistry
  • Chemical Kinetics
  • Molecular Spectroscopy

Background:

  • Excited states play a crucial role in photochemical reactions.
  • Understanding the competition between radiative and radiationless decay pathways is essential for controlling reaction outcomes.
  • Electron transfer and locally excited states exhibit distinct photophysical behaviors.

Purpose of the Study:

  • To investigate the factors controlling radiative and radiationless decay processes in excited states.
  • To quantitatively describe radiationless decay rate constants as a function of charge transfer.
  • To elucidate the mechanisms governing excited states with intermediate charge-transfer character.

Main Methods:

  • Studied excited states formed by cyanoanthracene acceptors and alkylbenzene donors.

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  • Utilized solvents of moderate to low polarity.
  • Measured rate constants for radiative decay, radiationless decay, and intersystem crossing.

    • Main Results:

    • Reported rate constants for radiative decay, radiationless decay, and intersystem crossing.
    • Observed excited states ranging from pure electron transfer to pure locally excited.
    • Demonstrated that radiationless decay rate constants can be quantitatively described by a weighted combination of locally excited and electron-transfer mechanisms.

    Conclusions:

    • The extent of charge transfer fundamentally influences the relative efficiencies of radiative and radiationless decay.
    • A model incorporating contributions from locally excited and electron-transfer mechanisms accurately predicts radiationless decay rates.
    • Factors controlling radiationless decay in states with intermediate charge transfer were elucidated.