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Time-dependent fluorescence spectra of large molecules in polar solvents

Hsu, Chao-Ping and Georgievskii, Yuri and Marcus, R. A. (1998) Time-dependent fluorescence spectra of large molecules in polar solvents. Journal of Physical Chemistry A, 102 (16). pp. 2658-2666. ISSN 1089-5639. http://resolver.caltech.edu/CaltechAUTHORS:20150609-082842994

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Abstract

A method is described for incorporating the vibronic transitions of a solute molecule in the calculation of the time evolution of its fluorescence spectrum in a polar solvent. In this initial article, systems are treated in which the intramolecular vibrational relaxation is much faster than the observed delay time. The overall fluorescence spectrum is then shown to be a convolution of the steady-state absorption and emission spectra of the solute in a nonpolar solvent and the time-dependent emission line shape arising only from polar interactions. Calculations are made for coumarin 153 in acetonitrile, using the dielectric dispersion data of the solvent available from experimental measurements. The results are in encouraging agreement with experimental spectra. Results are also given for the dynamic Stokes shift in methanol.


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http://dx.doi.org/10.1021/jp980255n DOIArticle
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Additional Information:© 1998 American Chemical Society. Received: November 19, 1997. We wish to particularly thank Professor J. E. Bertie for providing the data file and the computer code on the dielectric dispersion of acetonitrile before publication. It is a pleasure to acknowledge the support of the National Science Foundation and the Office of Naval Research. Y.G. would like to acknowledge the support of the James W. Glanville Postdoctoral Scholarship in Chemistry at Caltech and the support in the early stages of this research by a Rueff-Wormser Fellowship.
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NSFUNSPECIFIED
Office of Naval Research (ONR)UNSPECIFIED
James W. Glanville Postdoctoral ScholarshipUNSPECIFIED
Rueff-Wormser FellowshipUNSPECIFIED
Record Number:CaltechAUTHORS:20150609-082842994
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20150609-082842994
Official Citation:Time-Dependent Fluorescence Spectra of Large Molecules in Polar Solvents Chao-Ping Hsu,Yuri Georgievskii, and R. A. Marcus The Journal of Physical Chemistry A 1998 102 (16), 2658-2666 DOI: 10.1021/jp980255n
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ID Code:58101
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:09 Jun 2015 15:53
Last Modified:09 Jun 2015 15:53

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