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Ultrafast light-induced molecular reactions on aerosolized nanoparticles may elucidate early steps in the photoactivity of nanoparticles with potential impact in fields ranging from chemistry and medicine to climate science. In situ morphology discrimination for nanoparticle streams when measuring light-induced reaction yields is crucial, but lacking. Here, we experimentally demonstrate, using the reaction nanoscopy technique, that proton momenta from deprotonation reactions induced by intense femtosecond pulses exhibit clear, distinguishable signatures for single silica nanospheres and their clusters. Our findings are supported by classical trajectory Monte Carlo simulations. The results demonstrate an in situ single-shot discrimination method between reaction yields from photoinduced processes on single particles and their clusters. We find that the ionization of clusters dominates at sufficiently low intensities, providing an explanation to resolve previously observed discrepancies between experimental data and theoretical treatments, which considered only single nanoparticles.

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We present the results of a systematic study of photoelectron emission from gasphase dielectric nanoparticles (SiO 2 ) irradiated by intense 25 fs, 780 nm linearly polarized laser pulses as a function of particle size (20 nm to 750 nm in diameter) and laser intensity. We also introduce an experimental technique to reduce the effects of focal volume averaging. The highest photoelectron energies show a strong size dependence, increasing by a factor of six over the range of particles sizes studied at a fixed intensity. For smaller particle sizes (up to 200 nm), our findings agree well with earlier results obtained with few-cycle, ~4 fs pulses. For large nanoparticles, which exhibit stronger near-field localization due to field-propagation effects, we observe the emission of much more energetic electrons, reaching energies up to ~200 times the ponderomotive energy. This strong deviation in maximum photoelectron energy is attributed to the increase in ionization and charge interaction for many-cycle pulses at similar intensities.

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Strong-field laser-matter interactions in nanoscale targets offer unique avenues for the generation and detailed characterization of matter under extreme conditions. Field-driven, subcycle ionization-induced metallization of nanoscale solids in intense laser fields has been predicted (Peltz et al. Time-Resolved X-ray Imaging of Anisotropic Nanoplasma Expansion. Phys. Rev. Lett. 2014, 113, 133401), but its observation was hampered by a lack of a smoking gun. Here, we report the ultrafast metallization of isolated dielectric and semiconducting nanoparticles under intense few-cycle laser pulses. The highest-energy electron emission is found to be a decisive proof that shows a characteristic cutoff modification to a metallic limit for intensities high enough to ignite carrier avalanching in the volume of the particles. Semiclassical Mean-field Mie Monte-Carlo transport simulations reveal the underlying dynamics and explain the observed evolution by near-field driven electron backscattering from the metallizing target.

The development of attosecond metrology has enabled time-resolved studies on atoms, molecules, and (nanostructured) solids. Despite a wealth of theoretical work, attosecond experiments on isolated nanotargets, such as nanoparticles, clusters, and droplets have been lacking. Only recently, attosecond streaking metrology could be extended to isolated silica nanospheres, enabling real-time measurements of the inelastic scattering time in dielectric materials. Here, we revisit these experiments and describe the single-shot analysis of velocity-map images, which permits to evaluate the recorded number of electrons. Modeling of the recorded electron histograms allows deriving the irradiated nanoparticle statistics. Theoretically, we analyze the influence of the nanoparticle size on the field-induced delay, which is one of the terms contributing to the measured streaking delay. The obtained new insight into attosecond streaking experiments on nanoparticles is expected to guide wider implementation of the approach on other types of nanoparticles, clusters, and droplets.

In this paper, the effect of laser pulse energy on orthogonal double femtosecond pulse laser induced breakdown spectroscopy (LIBS) in air is studied. In the experiment, the energy of the probe pulse is changeable, while the pump pulse energy is held constant. At the same time, a systematic study of the laser induced breakdown spectroscopy signal dependence on the inter-pulse delay between the two pulses is performed. It is noted that the double pulse orthogonal configuration yields 2-32 times signal enhancement for the ionic and atomic lines as compared to the single pulse LIBS spectra when an optimum temporal separation between the two pulses is used, while there is no significant signal enhancement for the molecular lines in the studied range of the delay. It is also noted that the dependence of the enhancement factor for ionic and atomic lines on the inter-pulse delay can be fitted by Gaussian function. Furthermore, the electron temperature obtained by the relative line-to-continuum intensity ratio method was used to explain the LIBS signal enhancement.