We report on the formation of high-density regular arrays of nanometer-scale rods using femtosecond laser irradiation of a silicon surface immersed in water. The resulting surface exhibits both micrometer-scale and nanometer-scale structures. The micrometer-scale structure consists of spikes of 5-10 mum width, which are entirely covered by nanometer-scale rods that are roughly 50 nm wide and normal to the surface of the micrometer-scale spikes. The formation of the nanometer-scale rods involves several processes: refraction of laser light in highly excited silicon, interference of scattered and refracted light, rapid cooling in water, roughness-enhanced optical absorptance, and capillary instabilities.

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We have developed a femtosecond single-shot spectroscopic technique to measure irreversible changes in condensed phase materials in real time. Crossed echelons generate a two-dimensional array of time-delayed pulses with one femtosecond probe pulse. This yields 9 ps of time-resolved data from a single laser shot, filling a gap in currently employed measurement methods. We can now monitor ultrafast irreversible dynamics in solid-state materials or other samples that cannot be flowed or replenished between laser shots, circumventing limitations of conventional pump-probe methods due to sample damage or product buildup. Despite the absence of signal-averaging in the single-shot measurement, an acceptable signal-to-noise level has been achieved via background and reference calibration procedures. Pump-induced changes in relative reflectivity as small as 0.2%-0.5% are demonstrated in semimetals, with both electronic and coherent phonon dynamics revealed by the data. The optical arrangement and the space-to-time conversion and calibration procedures necessary to achieve this level of operation are described. Sources of noise and approaches for dealing with them are discussed.