Second- and third-harmonic generation as a local probe for nanocrystal-doped polymer materials with a suppressed optical breakdown threshold

摘要

Second- and third-harmonic generation processes are shown to allow the detection of absorptive agglomerates of nanocrystals in transparent materials and the visualization of optical breakdown in nanocomposite materials. Correlations between laser-induced breakdown and the behavior of the second- and third-harmonic signals produced in SiC/PMMA nanocomposite films are studied. The potential of second- and third-harmonic generation for the on-line visualization of laser breakdown in nanocomposite polymer materials is revealed, with the ablative material removal being monitored by the decay of the second- and third-harmonic signals. The second and third harmonics generated around the optical breakdown threshold by 75-fs pulses of 1.25-μm Cr:forsterite laser radiation are respectively more than two and four orders of magnitude more intense than the second and third harmonics produced under identical conditions by 40-ps pulses of a Nd:YAG laser. The breakdown threshold for PMMA films doped with 10-20-nm SiC nanocrystals forming absorptive agglomerates are demonstrated to be more than an order of magnitude lower than the breakdown threshold for crystalline SiC and about an order of magnitude lower than that for nondoped PMMA films.