Early stages of pulsed-laser growth of silicon microcolumns and microcones in air and SF6

Dense arrays of high-aspect-ratio silicon microcolumns and microcones are formed by cumulative nanosecond pulsed excimer laser irradiation of single-crystal silicon in oxidizing atmospheres such as air and SF6. Growth of such surface microstructures requires a redeposition model and also involves elements of self-organization. The shape of the microstructures, i.e., straight columns vs. steeply sloping cones and connecting walls, is governed by the type and concentration of the oxidizing species, e.g., oxygen vs. fluorine. Growth is believed to occur by a ''catalyst-free" VLS (vapor-liquid-solid) mechanism that involves repetitive melting of the tips of the columns/cones and deposition there of the ablated flux of Si-containing vapor. Results are presented of a new investigation of how such different final microstructures as microcolumns or microcones joined by walls nucleate and develop. The changes in silicon surface morphology were systematically determined and compared as the number of pulsed KrF (248 nm) laser shots was increased from 25 to several thousand in both air and SF6. The experiments in air and SF6 reveal significant differences in initial surface cracking and pattern formation. Consequently, local protrusions are first produced and column or cone/wall growth is initiated by different processes and at different rates. Differences in the spatial organization of column or cone/wall growth also are apparent. (C) 2000 Elsevier Science B.V. All rights reserved.