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Electronic energy transfer on CaO surfaces.

Alan G Joly¹, Kenneth M Beck, Wayne P Hess

¹Pacific Northwest National Laboratory, P.O. Box 999, Richland, Washington 99352, USA.

The Journal of Chemical Physics

|December 3, 2008

Summary

This study reveals that UV laser pulses trigger oxygen atom emission from nanostructured calcium oxide (CaO) via an electronic excited-state desorption mechanism, with yield increasing below the bulk absorption threshold.

Area of Science:

Surface Science
Materials Chemistry
Laser-Induced Desorption

Background:

Nanostructured metal oxides exhibit unique surface properties.
Understanding surface reactions is crucial for catalysis and materials science.
Laser-induced desorption provides insights into surface electronic states.

Purpose of the Study:

To investigate the mechanism of hyperthermal O-atom emission from nanostructured CaO.
To explore the role of electronic excited states in laser desorption.
To analyze the photon energy dependence of O-atom yield and kinetic energy.

Main Methods:

Excitation of nanostructured CaO with tunable UV laser pulses.
Detection and analysis of hyperthermal O-atom emission.

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Application of a laser desorption model developed for nanostructured MgO.

Main Results:

Hyperthermal O-atom emission was observed, indicating an electronic excited-state desorption mechanism.
O-atom yield increased significantly with photon energy (3.75–5.4 eV), below the bulk absorption threshold.
Peak kinetic energy of O-atoms remained constant with increasing photon energy (3.9–5.15 eV).

Conclusions:

The results support a model of desorption induced by exciton localization at corner-hole trapped surface sites.
Electronic energy transfer from higher coordinated surface sites plays a role in the observed desorption.
The findings offer insights into laser-surface interactions on nanostructured oxides.