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We use intense femtosecond extreme ultraviolet (XUV) pulses with a photon energy of 92 eV from the FLASH free electron laser to irradiate substrate-free CsCl nanoparticles surrounded by a He gas with a number density of around 10 ^15 cm ^−3 . By simultaneously detecting electrons and energetic ions from the laser-irradiated micron-size target we study the acceleration mechanism of light ions at the microplasma-vacuum boundary as well as at the layer close to the nanoparticle surface. When the XUV pulse interacts with the gas alone, helium ions are accelerated to energies exceeding 100 eV. In the presence of the nanoparticle, light ions gain additional energy in the electric field around the ionized nanoparticle and their energy spectrum changes considerably. We present an electrostatic model to explain the ion acceleration mechanisms both with and without the nanoparticle and discuss the role of the gas environment in experiments.

We have investigated the possibility to track and control correlation dynamics of valence electrons in krypton (Kr) initiated by the absorption of one extreme ultraviolet (XUV) photon. In this investigation, pump-probe experiments have been performed where monochromatized single high-harmonics at photon energies 29.6, 32.8, and 35.9 eV have been used as pump to populate different intermediate excited states. A temporally delayed near-infrared (NIR) pulse probes the population of various decay channels via the detection of Kr ^2+ ion yields and its transient profiles. We observe that by varying the NIR pulse intensity within a range from $0.3\times10^{13}$ to $2.6\times10^{13}$ W cm ^−2 , the shape of the Kr ^2+ transient profile changes significantly. We show that by varying the intensity of the NIR pulse, it is possible—(i) to control the ratio between sequential and non-sequential double ionization of Kr; (ii) to selectively probe quantum beating oscillations between Kr $^{+*}$ satellite states that are coherently excited within the bandwidth of the XUV pulse; and (iii) to specifically probe the relaxation dynamics of doubly excited (Kr $^{**}$ ) decay channels. Our studies show that the contribution of different ionization and decay channels (i)–(iii) can be altered by the NIR pulse intensity, thus demonstrating an efficient way to control the ionization dynamics in rare gas atoms.

Many linked processes occur concurrently in strongly excited semiconductors, such as interband and intraband absorption, scattering of electrons and holes by the heated lattice, Pauli blocking, bandgap renormalization and the formation of Mahan excitons. In this work, we disentangle their dynamics and contributions to the optical response of a ZnO thin film. Using broadband pump-probe ellipsometry, we can directly and unambiguously obtain the real and imaginary part of the transient dielectric function which we compare with first-principles simulations. We find interband and excitonic absorption partially blocked and screened by the photo-excited electron occupation of the conduction band and hole occupation of the valence band (absorption bleaching). Exciton absorption turns spectrally narrower upon pumping and sustains the Mott transition, indicating Mahan excitons. Simultaneously, intra-valence-band transitions occur at sub-picosecond time scales after holes scatter to the edge of the Brillouin zone. Our results pave new ways for the understanding of non-equilibrium charge-carrier dynamics in materials by reliably distinguishing between changes in absorption coefficient and refractive index, thereby separating competing processes. This information will help to overcome the limitations of materials for high-power optical devices that owe their properties from dynamics in the ultrafast regime.