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Adsorption-state-dependent subpicosecond photoinduced desorption dynamics.

Paul Szymanski¹, Alex L Harris, Nicholas Camillone

¹Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973-5000.

The Journal of Chemical Physics

|June 15, 2007

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Femtosecond laser pulses reveal how molecular oxygen desorbs from palladium surfaces. The study shows desorption efficiency depends on oxygen

Area of Science:

Surface Science
Physical Chemistry
Femtochemistry

Background:

Understanding substrate-adsorbate coupling is crucial for surface reactions.
Femtosecond laser excitation probes ultrafast dynamics at surfaces.
Molecular oxygen adsorbs on Pd(111) in distinct peroxo and superoxo states.

Purpose of the Study:

To investigate the adsorption-state dependence of substrate-adsorbate coupling during molecular oxygen desorption from Pd(111).
To elucidate the mechanism of photoinduced desorption using femtosecond laser pulses.
To correlate desorption dynamics with coverage and electronic states.

Main Methods:

Femtosecond laser excitation to initiate desorption of molecular oxygen (O2) from Pd(111).
Two-pulse correlation measurements to probe ultrafast dynamics.

Related Experiment Videos

Varying O2 coverage to alter the relative populations of peroxo (O2(2-)) and superoxo (O2-) states.

Main Results:

A dominant 400 fs response and a slower 10 ps decay were observed, largely independent of O2 coverage.
Photodesorption yield and fluence dependence showed a clear coverage dependence.
Superoxo states exhibit greater desorption efficiency than peroxo states.

Conclusions:

Photoinduced desorption is primarily driven by an electron-mediated mechanism common to both states.
The electron-phonon two-temperature model with adsorbate-electron frictional coupling successfully reproduces experimental trends.
A transition from diabatic to adiabatic regimes explains the biexponential correlation behavior.