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This study reveals a shift in how C60 molecules ionize under intense femtosecond laser fields. Ionization from superatom molecular orbitals transitions to Rydberg states as laser intensity increases.

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Area of Science:

  • Physical Chemistry
  • Quantum Mechanics
  • Materials Science

Background:

  • Fullerenes like C60 exhibit complex ionization dynamics under intense laser fields.
  • Understanding these dynamics is crucial for applications in laser-matter interactions and materials modification.

Purpose of the Study:

  • To investigate the transition between different ionization mechanisms in C60 molecules using femtosecond laser pulses.
  • To characterize the dominant ionization pathways as a function of laser intensity.

Main Methods:

  • Femtosecond laser spectroscopy at 785 nm with intensities ranging from 3 to 20 TW/cm2.
  • Velocity map imaging to obtain electron kinetic energy spectra.
  • Time-dependent density functional theory (TD-DFT) simulations for spectral assignment.

Main Results:

  • Observed a transition in ionization mechanisms for C60 molecules.
  • Ionization from superatom molecular orbitals (SAMOs) dominates at lower intensities (< 5 TW/cm2).
  • Ionization from Rydberg states becomes more prominent at higher intensities, with evidence of over-the-barrier ionization from f-Rydberg states.

Conclusions:

  • The ionization mechanism in C60 is strongly dependent on laser intensity.
  • TD-DFT simulations successfully assigned spectral features to SAMOs and Rydberg states.
  • Distinct photoelectron angular distributions provide insights into shallow f-Rydberg state ionization.