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Ch Zaum1, K M Meyer-Auf-der-Heide1, M Mehlhorn1

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Summary
This summary is machine-generated.

Femtosecond laser excitation reveals surprising oscillatory energy dependence in carbon monoxide (CO) diffusion on copper surfaces. Laser-driven diffusion shows an inverted phase compared to thermal diffusion, explained by transient negative ion stabilization.

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Area of Science:

  • Surface science
  • Physical chemistry
  • Femtosecond spectroscopy

Background:

  • Understanding molecule diffusion on surfaces is crucial for catalysis and materials science.
  • Carbon monoxide (CO) diffusion on metal surfaces like copper (Cu) is a fundamental process.
  • Investigating long-range interactions during diffusion can reveal novel mechanisms.

Purpose of the Study:

  • To investigate the long-range interaction during carbon monoxide (CO) diffusion on a Cu(111) surface.
  • To compare the energy dependence of thermal and laser-driven diffusion.
  • To elucidate the underlying mechanism for observed diffusion behaviors.

Main Methods:

  • Utilizing femtosecond laser excitation combined with a low-temperature scanning tunneling microscope (STM).
  • Studying the diffusion of CO molecules on a well-defined Cu(111) surface.
  • Performing ab initio calculations to support experimental findings.

Main Results:

  • Both thermal and laser-driven CO diffusion exhibit oscillatory energy dependence on the distance to neighboring molecules.
  • An unexpected inverted phase relationship was observed between thermal and laser-driven diffusion.
  • Laser-driven diffusion is facile at distances where thermal diffusion is hindered, and vice versa.

Conclusions:

  • The inverted phase in diffusion is attributed to transient stabilization of the CO negative ion during laser excitation.
  • Femtosecond laser excitation provides a unique pathway to control and study surface diffusion dynamics.
  • This study offers new insights into molecule-surface interactions and non-thermal diffusion mechanisms.