Femtosecond time-resolved laser-induced desorption of positive ions from MgO

We have used the pump-probe technique to measure the photostimulated positive ion yield as a funct:ion of time delay between two sub-threshold femtosecond laser pulses. We find that the ion yield from UV femtosecond irradiated MgO depends critically on the laser pulse delay, Delta t, in two-pulse experiments. In single-pulse experiments, excitation of MgO produces a variety of ions including Mg+, MgO+, and a significant yield of H+. In contrast, if the femtosecond laser pulse is split into two sub-threshold beams and then recombined with a variable time delay, the ion yield may be drastically altered depending on the delay between pulses. The Mg+ desorption yield displays three distinct lifetimes and persists for laser delays of over 100 ps. A pulse delay of only Delta t = 500 fs nearly eliminates ion desorption except for Mg+. The use of a pair of delayed femtosecond laser pulses can thus control the species of the desorbed ion. The mechanism for femtosecond laser desorption is clearly different from nanosecond laser desorption. We hypothesize that the creation of electron-hole pairs by nonresonant two-photon excitation contributes to the ultrafast desorption mechanism.