Ultrafast relaxation of fullerenes and fullerites by broadband femtosecond laser spectrometry

Daniel Boucher; Sergey V. Chekalin; S. A. Kovalenko; Juru A. Matveets; P. Masselin; M. G. Novikov; V. V. Ragulsky; Andrei G. Stepanov

doi:10.1117/12.287696

26 September 1997 Ultrafast relaxation of fullerenes and fullerites by broadband femtosecond laser spectrometry

Daniel Boucher, Sergey V. Chekalin, S. A. Kovalenko, Juru A. Matveets, P. Masselin, M. G. Novikov, V. V. Ragulsky, Andrei G. Stepanov

Author Affiliations +

Proceedings Volume 3239, Photon Echo and Coherent Spectroscopy; (1997) https://doi.org/10.1117/12.287696
Event: PECS '97: Photon Echo and Coherent Spectroscopy, 1997, Yoshkar-Ola, Russian Federation

Abstract

Relaxation of fullerenes in solids and solutions was investigated by femtosecond pump-probe technique at various experimental setups. Intensity of excitation pulse was varied at 10¹⁰ - 10¹² W/cm², energies of pump and probe quanta were changed from 1.57 to 3.14 eV, pulse duration -- from 60 to 350 fs. An increase of absorption was observed in solutions with a time scale of 1.2 ps for C₆₀ and 0.15 ps for C₇₀ after excitation of HOMO-LUMO transition. It was attributed to symmetry breaking of excited molecules. Observed for solid C₆₀ dependence of relaxation rate on the density of excited molecules and on the wavelengths of the pump and probe pulses is explained by 'hot' singlet-singlet annihilation the rate of which is proportional to R^-3. Comparison of photoinduced absorption and bleaching decays allowed to conclude that only a small fracture of excited molecules produce localized charge carriers, mainly by excitonic annihilation proces and these carriers are responsible for long-lived residual absorption observed in photoinduced absorption kinetics. Difference absorption spectra observed near zero delay time were similar to electroabsorption ones superimposed on excited state absorption of C₆₀ film. This electroabsorption feature disappeared in phase with pumping pulse. This phenomenon is connected with Stark shift in strong electric field of the powerful pumping pulse.

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Daniel Boucher, Sergey V. Chekalin, S. A. Kovalenko, Juru A. Matveets, P. Masselin, M. G. Novikov, V. V. Ragulsky, and Andrei G. Stepanov "Ultrafast relaxation of fullerenes and fullerites by broadband femtosecond laser spectrometry", Proc. SPIE 3239, Photon Echo and Coherent Spectroscopy, (26 September 1997); https://doi.org/10.1117/12.287696

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