Mass removed from single crystal silicon samples by high irradiance (1×109 to 1×1011 W/cm2) single pulse laser ablation was studied by measuring the resulting crater morphology with a white light interferometric microscope. The craters show a strong nonlinear change in both the volume and depth when the laser irradiance is less than or greater than ≈2.2×1010 W/cm2. Time-resolved shadowgraph images of the ablated silicon plume were obtained over this irradiance range. The images show that the increase in crater volume and depth at the threshold of 2.2×1010 W/cm2 is accompanied by large size droplets leaving the silicon surface, with a time delay ∼300 ns. A numerical model was used to estimate the thickness of the layer heated to approximately the critical temperature. The model includes transformation of liquid metal into liquid dielectric near the critical state (i.e., induced transparency). In this case, the estimated thickness of the superheated layer at a delay time of 200–300 ns shows a close agreement with measured crater depths. Induced transparency is demonstrated to play an important role in the formation of a deep superheated liquid layer, with subsequent explosive boiling responsible for large-particulate ejection.

The craters resulting from high-irradiance (1×109–1×1011 W/cm2) single-pulse laser ablation of single-crystal silicon show a dramatic increase in volume at a threshold irradiance of 2.2×1010 W/CM2. Time-resolved shadowgraph images show ejection of large particulates from the sample above this threshold irradiance, with a time delay ∼300 ns. A numerical model was used to estimate the thickness of a superheated layer near the critical state. Considering the transformation of liquid metal into liquid dielectric near the critical state (i.e., induced transparency), the calculated thickness of the superheated layer at a delay time of 200–300 ns agreed with the measured crater depths. This agreement suggests that induced transparency promotes the formation of a deep superheated layer, and explosive boiling within this layer leads to particulate ejection from the sample.

The relation between laser-generated particles and ICPMS signal intensity was investigated using single-pulse laser ablation sampling of solids. The particle size distribution of glass samples was measured using an optical particle counter for different laser ablation conditions. Ablation of a new surface produced fewer particles and lower ICPMS signal intensity than a preablated surface. Laser power density of 0.4−0.5 GW/cm2 was found to be a threshold value, across which particle size distribution changed. Laser beam diameter was a more influential parameter than power density in efficient particle generation. Particle loss during transport from the ablation chamber to the ICPMS was significant for a low carrier gas flow rate of 0.1 L/min, while almost no loss was observed for a higher flow rate of 0.26 L/min. The onset of ICPMS intensity time profiles decreased as more large particles were generated. ICPMS intensity data were calibrated with respect to the particle mass entering the ICPMS. Particle entrainment efficiency of the LA-ICPMS system was estimated and found to be a strong function of laser power density.

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