Attosecond dynamics of nano-localized fields probed by photoelectron spectroscopy

摘要

This work focuses on the interaction of few-cycle laser pulses with nanosystems. Special emphasis is placed on the spatio-temporal evolution of the induced near-fields. Measurements on carrier-envelope-phase (CEP) controlled photoemission from isolated SiO2 nanospheres are taken by single-shot velocity map imaging (VMI) combined with CEP tagging. The obtained photoelectron spectra show a pronounced dependence on the CEP and extend to unexpectedly high energies. Comparison with numerical simulations identify the additional Coulomb forces of the liberated electron cloud as an effective additional acceleration mechanism for distinct trajectories. For larger spheres, an asymmetry in the field distribution is classically predicted. This asymmetry is also observed in the photoelectron momentum distributions. The mapping between position and momentum space in the VMI approach are investigated by analyzing the correlation of the photoelectron's birth and detection position.ududIn a second set of experiments, photoemission at intensities exceeding 10^14 W/cm^2 from isolated nanospheres of different composition (SiO2, ZrO2, TiO2, Si, Au) is examined by stereo time-of-flight spectroscopy. It is found that the measured cutoff energies scale non-linearly with laser intensity depending on the material properties of the nanosystem. A trend towards a unified behavior for high intensities is observed indicating a drastic change in optical properties within the duration of the few-cycle laser pulse. The charge carrier generation mechanisms that could lead to such a transient effect are discussed.ududFor a better understanding of the interaction of few-cycle fields with nanosystems, a direct access to the temporal evolution of (plasmonic) near-fields is highly desirable. The efforts on the realization of nanoplasmonic attosecond streaking spectroscopy are presented. Numerical simulations are used to identify the influence of the inhomogeneous near-field distributions on the streaking process. First experimental results obtained from Au nanotips show clear streaking features of sub-micron localized near-fields. The near-field oscillations are found to be phase offset as compared to reference measurements. The exact origin of the streaking features of the Au tip and possible improvements of the experimental approach are discussed.