Low-order harmonic generation in nanosecond laser ablation plasmas of carbon containing materials

In this work we report on a systematic study of the spatiotemporal behaviour of low-order harmonics generated in nanosecond laser ablation plasmas of carbon containing materials. Plasmas were generated from targets of graphite and boron carbide ablated with a nanosecond Q-switched Nd:YAG laser at 1064 nm. Low-order harmonics (3rd and 5th) of the fundamental wavelength of a ns Nd:YAG driving laser, propagating perpendicularly to the ablation laser at variable time delays, were observed. The temporal study of the low-order harmonics generated under vacuum and atmospheres of Kr and Xe, revealed the presence of two populations that contribute to the harmonic generation (HG) at different times. It was found that under vacuum only small species contribute to the HG process, whereas under buffer gas, heavier species, such as clusters and nanoparticles, contribute to the HG at longer times. Optical emission spectroscopy, time of flight mass spectrometry and characterization of deposits collected on-line on a nearby substrate provided additional information that complemented the results of the spatiotemporal study of the generated harmonics. This approach to ablation plume analysis allows elucidating the identity of the nonlinear emitters in laser ablation plasmas and facilitates the investigation of efficient, nanoparticle-enhanced, coherent short wavelength generation processes.