Research on Chemical Intermediates

, Volume 23, Issue 7, pp 587–600 | Cite as

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

  • V. Klimov
  • L. Smilowitz
  • H. Wang
  • M. Grigorova
  • J. M. Robinson
  • A. Koskelo
  • B. R. Mattes
  • F. Wudl
  • D. W. McBranch
Article

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.

Keywords

Fullerene Probe Pulse Transient Absorption Relaxation Dynamic Transient Absorption Spectrum 

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Copyright information

© Springer 1997

Authors and Affiliations

  • V. Klimov
    • 1
  • L. Smilowitz
    • 1
  • H. Wang
    • 2
  • M. Grigorova
    • 1
  • J. M. Robinson
    • 1
  • A. Koskelo
    • 1
  • B. R. Mattes
    • 1
  • F. Wudl
    • 2
  • D. W. McBranch
    • 1
  1. 1.Chemical Science and Technology DivisionLos Alamos National LaboratoryLos AlamosUSA
  2. 2.Institute for Polymers and Organic SolidsUniversity of CaliforniaSanta BarbaraUSA

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