Femtosecond to nanosecond dynamics in fullerenes: Implications for excitedstate optical nonlinearities

Victor I Klimov, L. Smilowitz, H. Wang, M. Grigorova, J. M. Robinson, A. Koskelo, B. R. Mattes, F. Wudl, D. W. McBranch

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23 Citations (Scopus)

Abstract

We compared detailed dynamics of the excited-state absorption for C60 in solution, thin films, and entrapped in an inorganic sol-gel glass matrix. Our results demonstrate that the microscopic morphology of the C60 molecules plays a crucial role in determining the relaxation dynamics. This is a key factor for applications in optical limiting for nanosecond pulses using reverse saturable absorption. We find that the dynamics of our C60-glass composites occur on long (ns) timescales, comparable to those in solution; thin film samples, by contrast, show rapid decay (60-sol-gel glass composites contain C60 in a molecular dispersion, and are suitable candidates for solid-state optical limiting. Multispectral analysis of the decay dynamics in solution allows accurate determination of both the intersystem crossing time (600±100ps) and the relative strengths of the singlet and triplet excited-state cross sections as a function of wavelength from 450-950 nm. The triplet excited-state cross section is greater than that for the singlet excited-state over the range from 620-810 nm.

Original languageEnglish
Pages (from-to)587-600
Number of pages14
JournalResearch on Chemical Intermediates
Volume23
Issue number7
DOIs
Publication statusPublished - Jul 1997

ASJC Scopus subject areas

  • Chemistry(all)

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    Klimov, V. I., Smilowitz, L., Wang, H., Grigorova, M., Robinson, J. M., Koskelo, A., Mattes, B. R., Wudl, F., & McBranch, D. W. (1997). Femtosecond to nanosecond dynamics in fullerenes: Implications for excitedstate optical nonlinearities. Research on Chemical Intermediates, 23(7), 587-600. https://doi.org/10.1163/156856797X00024