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

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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 (<20 picoseconds). These results demonstrate that C60-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.

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Authors and Affiliations

  1. Chemical Science and Technology Division, Los Alamos National Laboratory, 87545, Los Alamos, NM, USA

    V. Klimov, L. Smilowitz, M. Grigorova, J. M. Robinson, A. Koskelo, B. R. Mattes & D. W. McBranch

  2. Institute for Polymers and Organic Solids, University of California, 93106, Santa Barbara, CA, USA

    H. Wang & F. Wudl

Authors
  1. V. Klimov
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  2. L. Smilowitz
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  3. H. Wang
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  4. M. Grigorova
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  5. J. M. Robinson
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  6. A. Koskelo
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  7. B. R. Mattes
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  8. F. Wudl
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  9. D. W. McBranch
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Klimov, V., Smilowitz, L., Wang, H. et al. Femtosecond to nanosecond dynamics in fullerenes: Implications for excitedstate optical nonlinearities. Res. Chem. Intermed. 23, 587–600 (1997). https://doi.org/10.1163/156856797X00024

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  • DOI: https://doi.org/10.1163/156856797X00024

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