Theory of Excited State Dynamics as Studied by Fourier Transform of Optical Absorption Spectra of Molecular Solutions
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For the purpose of analyzing the very rapid (tens to hundreds of femto-second)dynamics in the excited state of molecular solutions, we have derived an equation ofmotion for the time-correlation function of the transition dipole moment, which isrelated to an optical absorption spectrum by a Fourier transformation. We have solv-ed the above equation in the case of weak solute-solvent interaction, assuming theGauss process for field-fluctuation and force-fluctuation applied to the vibration of asolute molecule by the random collision of solverut molecules and by anharmonicvibration. By means of a systematic analysis of the absolute value and the phase angleof the time-correlation function, we can separate the properties of the intrinsic, ex-cited state dynamics from the field-fluctuation effect. We have exemplified how thedynamical relaxation parameters are evaluated from the experimentally obtained ab-sorption band 'A..='B.. of dilute benzene solutions.
- 社団法人日本物理学会の論文
- 1986-03-15
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