Relaxation Dynamics of Electronically Excited C60 in o-Dichlorobenzene and Tetrahydrofuran Solution

Helge Brands 1 , 1 , Oli T. Ehrler 2 , 2 , Manfred Kappes 3 , 3  and Andreas-Neil Unterreiner 4 , 4
  • 1  Paul Scherrer Institute, WBGB/013, Villigen PSI, Schweiz
  • 2  Carl Zeiss SMT GmbH, Laser Optics GmbH, Oberkochen, Deutschland
  • 3  Karlsruhe Institute of Technology, Institute for Physical Chemistry, Karlsruhe, Deutschland
  • 4  Karlsruher Institut für Technologie, Institut für Physikalische Chemie, Karlsruhe, Deutschland

Abstract

The ultrafast response of singly negatively charged C60 fullerene in solution has been investigated by femtosecond pump-probe absorption spectroscopy and transient anisotropy in the visible and near-infrared region. Pump excitation within the near-infrared band demonstrates that this spectral feature can be described as a vibrational progression associated with a single electronic transition. Relaxation of the first electronically excited state occurs primarily by internal conversion with a time constant of 3 ps, slightly depending on the solvents, tetrahydrofuran or o-dichlorobenzene, and also on the excitation wavelength. An excitation of the second electronically excited state around 530 nm leads to an ultrafast internal conversion to the first excited state with a pulse-limited time constant of less than 100 fs. As a minor channel, stimulated emission in the spectral regime of 1150–1300 nm was observed from the first electronically excited state both after near-infrared and visible excitation. After internal conversion to the electronic ground state, C60 dissipates its excess internal energy into the solvent on a longer timescale of 40–70 ps. The transient anisotropy associated with directly populating the first excited state reveals an ultrafast component decaying within 100 fs, which is attributed to ultrafast vibrational motions, conceivably arising from excited state pseudorotation.

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Founded in 1887, the Zeitschrift für Physikalische Chemie covers the main developments in physical chemistry, placing with an emphasis on experimental research. It represents a combination ofdiscusses reaction kinetics and spectroscopy, surface research and electrochemistry, thermodynamics and the structure analysis of matter in its various conditions, among other topics.

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