Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 1, Issue 12, Pages 1800-1804Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz100430x
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- Parma University
- U.S. Army Research Laboratory
- U.S. Army Research Office [50372-CH-MUR]
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Optical spectra of two families of symmetrical polymethine dyes bearing a positive and a negative charge are analyzed based on an essential state model recently developed for quadrupolar dyes. The model accounts for molecular vibrations and polar solvation and reproduces the anomalous evolution with solvent polarity of experimental absorption band shapes. Fluorescence and excited-state absorption spectra are well-described within the samle model which also quantitatively reproduces the recent observation of an intense two-photon absorption toward the (two-photon forbidden) lowest excited state. An extensive analysis of optical spectra demonstrates that the essential-state model developed for quadrupolar dyes also applies to polymethine dyes and that long polymethine dyes offer the first experimental example of class III quadrupolar chromophores.
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