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Area of Science:

  • Quantum physics
  • Materials science
  • Molecular electronics

Background:

  • Single-molecule electron sources, typically fullerenes (~1 nm), exhibit unusual emission patterns under constant electric fields.
  • These patterns, like crosses or two-leaf shapes, have remained unexplained for over 70 years.

Purpose of the Study:

  • To investigate the origin of peculiar electron emission patterns from single-molecule fullerene sources.
  • To explore the effect of femtosecond light pulses on these emission patterns.
  • To establish a link between emission patterns and molecular orbitals.

Main Methods:

  • Utilized single-molecule electron sources made of fullerenes.
  • Applied constant electric fields to drive electron emission.
  • Illuminated the sources with femtosecond laser pulses.
  • Performed theoretical simulations to analyze emission patterns.

Main Results:

  • Observed significantly modulated emission patterns upon illumination with femtosecond light pulses.
  • Simulations revealed that the emission patterns directly correspond to single-molecule molecular orbitals.
  • Demonstrated that modulations in patterns arise from dynamic variations in molecular orbitals.

Conclusions:

  • The long-standing mystery of fullerene electron emission patterns is solved, identifying them as molecular orbitals.
  • Achieved precise, subnanometric optical modulation of electron emission by controlling molecular orbitals.
  • Opens new avenues for advanced molecular electronic devices and nanoscale optical control.