Size-Dependent Ion Emission Asymmetry of Free NaCl Nanoparticles Excited by Intense Femtosecond Laser Pulses
We report on asymmetric ion emission of size-selected NaCl nanoparticles (d = 100 - 600 nm) ionized by intense femtosecond laser pulses (λ = 800 nm, peak intensity ~1013 W/cm2). Velocity map imaging indicates that a higher ion yield occurs in the propagation direction of the laser pulses than in opposite direction. This asymmetric ion emission is found to be size-dependent and increases with particle size. This pronounced size dependence is interpreted in terms of discrete dipole simulations of the internal electric field in the nanoparticles, which reveal that the internal field is enhanced in the forward propagation direction of the laser pulses, occurring for nanoparticles >100 nm. The ion emission asymmetry is further found to depend on the peak intensity of the laser radiation. Nanoparticles of 100 nm show a symmetric distribution of ion emission, while the ion emission for 600 nm particles is found to become increasingly symmetric as the peak intensity is increased. In addition to single pulse ionization experiments, we explore the angular distribution of ion emission of resonantly heated NaCl nanoparticles using a pump-probe setup. Here, ion emission is found to be more symmetric for resonantly heated nanoparticles than for single pulse excitation. These differences are explained by the absorption mechanism, where the probe pulse in a dual pulse experiment can be efficiently absorbed by plasmonic excitations for suitable delays between both laser pulses.