Primary processes of laser-induced selective dimer-layer removal on Si(001)-(2x1).

Excitation with nanosecond-laser pulses at fluences well below the melt threshold removes Si dimers on the Si(001)-(2x1) surface and induces atomic-Si desorption through an electronic mechanism. The rate of this photoinduced reaction depends superlinearly on the excitation intensity, and is enhanced resonantly at the photon energy where the optical transition injects holes into the dimer backbond surface-band state. The results reveal the crucial role of surface holes and their nonlinear localization in the bond rupture of Si dimers on this surface.