Clear observation of the formation of nanoparticles inside the ablation bubble through a laser-induced flat transparent window by laser scattering

To understand the formation mechanism of nanoparticles via laser ablation in liquids direct observation of the dynamics inside the ablation bubble is essential. One powerful technique for this is small-angle X-ray scattering. Applying the laser-scattering technique in a similar context faces some difficulties, because, firstly the probe laser does not easily go into the bubble due to the curved bubble surface, and secondly the extremely weak scattering signal from inside the bubble is overwhelmed by the very strong reflection at the bubble surface. In this paper we solve those two problems by sending the probe laser into the bubble through a laser-induced flat transparent window, and demonstrate the clean observation of laser-scattering signals from the inside of the ablation bubble. We observe the signature of the formation of nanoparticles around the two areas inside the bubble, i.e., around the central area and apex inside the bubble. The scattering signals originating from the centre of the bubble persist throughout the entire growth and shrinkage stages of the bubble, while practically no scattering signals are found outside the bubble and this clearly implies that almost all nanoparticles are formed inside the bubble. Interestingly, the scattering signals originating from the apex inside the bubble gradually emerge after the bubble reaches the maximum size, and they become brighter as it further shrinks. Those findings are consistent with the scenario of nanoparticle formation obtained by small-angle X-ray scattering experiments.