Attosecond Streaking in the Water Window: A New Regime of Attosecond Pulse Characterization

We report on the first streaking measurement of water-window attosecond pulses generated via high harmonic generation, driven by sub-2-cycle, CEP-stable, 1850 nm laser pulses. Both the central photon energy and the energy bandwidth far exceed what has been demonstrated thus far, warranting the investigation of the attosecond streaking technique for the soft X-ray regime and the limits of the FROGCRAB retrieval algorithm under such conditions. We also discuss the problem of attochirp compensation and issues regarding much lower photo-ionization cross sections compared with the XUV in addition to the fact that several shells of target gases are accessed simultaneously. Based on our investigation, we caution that the vastly different conditions in the soft X-ray regime warrant a diligent examination of the fidelity of the measurement and the retrieval procedure.Comment: 14 Pages, 12 figure

CO2\mathrm{CO_2} exploding clusters dynamics probed by XUV fluorescence

Clusters excited by intense laser pulses are a unique source of warm dense matter, that has been the subject of intensive experimental studies. The majority of those investigations concerns atomic clusters, whereas the evolution of molecular clusters excited by intense laser pulses is less explored. In this work we trace the dynamics of $\mathrm{CO_2}$ clusters triggered by a few-cycle 1.45-$\mu$m driving pulse through the detection of XUV fluorescence induced by a delayed 800-nm ignition pulse. Striking differences among fluorescence dynamics from different ionic species are observed

EUV ionization of pure He nanodroplets: Mass-correlated photoelectron imaging, Penning ionization and electron energy-loss spectra

The ionization dynamics of pure He nanodroplets irradiated by EUV radiation is studied using Velocity-Map Imaging PhotoElectron-PhotoIon COincidence (VMI-PEPICO) spectroscopy. We present photoelectron energy spectra and angular distributions measured in coincidence with the most abundant ions He+, He2+, and He3+. Surprisingly, below the autoionization threshold of He droplets we find indications for multiple excitation and subsequent ionization of the droplets by a Penning-like process. At high photon energies we evidence inelastic collisions of photoelectrons with the surrounding He atoms in the droplets

Penning ionization of doped helium nanodroplets following EUV excitation

Helium nanodroplets are widely used as a cold, weakly interacting matrix for spectroscopy of embedded species. In this work we excite or ionize doped He droplets using synchrotron radiation and study the effect onto the dopant atoms depending on their location inside the droplets (rare gases) or outside at the droplet surface (alkali metals). Using photoelectron-photoion coincidence imaging spectroscopy at variable photon energies (20-25 eV), we compare the rates of charge-transfer to Penning ionization of the dopants in the two cases. The surprising finding is that alkali metals, in contrast to the rare gases, are efficiently Penning ionized upon excitation of the (n=2)-bands of the host droplets. This indicates rapid migration of the excitation to the droplet surface, followed by relaxation, and eventually energy transfer to the alkali dopants

High-order harmonic spectroscopy for molecular imaging of polyatomic molecules

High-order harmonic generation is a powerful and sensitive tool for probing atomic and molecular structures, combining in the same measurement an unprecedented attosecond temporal resolution with a high spatial resolution, of the order of the angstrom. Imaging of the outermost molecular orbital by high-order harmonic generation has been limited for a long time to very simple molecules, like nitrogen. Recently we demonstrated a technique that overcame several of the issues that have prevented the extension of molecular orbital tomography to more complex species, showing that molecular imaging can be applied to a triatomic molecule like carbon dioxide. Here we report on the application of such technique to nitrous oxide (N2O) and acetylene (C2H2). This result represents a first step towards the imaging of fragile compounds, a category which includes most of the fundamental biological molecules

Ultrafast charge carrier dynamics in quantum confined 2D perovskite

We studied the charge carrier dynamics in 2D perovskite NBT2PbI4 by ultrafast optical pump-THz probe spectroscopy. We observed a few ps long relaxation dynamics that can be ascribed to the band to band carrier recombination, in the absence of any contribution from many-body and trap assisted processes. The transient conductivity spectra show that the polaron dynamics is strongly modulated by the presence of a rich exciton population. The polarization field resulting from the exciton formation acts as the source of a restoring force that localizes polarons. This is revealed by the presence of a negative imaginary conductivity. Our results show that the dynamics of excitons in 2D perovskites at room temperature can be detected by monitoring their effect on the conductivity of the photoinduced polaronic carrier

Collective Autoionization in Multiply-Excited Systems: A novel ionization process observed in Helium Nanodroplets

Free electron lasers (FELs) offer the unprecedented capability to study reaction dynamics and image the structure of complex systems. When multiple photons are absorbed in complex systems, a plasma-like state is formed where many atoms are ionized on a femtosecond timescale. If multiphoton absorption is resonantly-enhanced, the system becomes electronically-excited prior to plasma formation, with subsequent decay paths which have been scarcely investigated to date. Here, we show using helium nanodroplets as an example that these systems can decay by a new type of process, named collective autoionization. In addition, we show that this process is surprisingly efficient, leading to ion abundances much greater than that of direct single-photon ionization. This novel collective ionization process is expected to be important in many other complex systems, e.g. macromolecules and nanoparticles, exposed to high intensity radiation fields

Interatomic Coulombic decay in helium nanodroplets

Interatomic Coulombic decay (ICD) is induced in helium nanodroplets by photoexciting the n = 2 excited state of He + using XUV synchrotron radiation. By recording multiple-coincidence electron and ion images we find that ICD occurs in various locations at the droplet surface, inside the surface region, or in the droplet interior. ICD at the surface gives rise to energetic He + ions as previously observed for free He dimers. ICD deeper inside leads to the ejection of slow He + ions due to Coulomb explosion delayed by elastic collisions with neighboring He atoms, and to the formation of He k + complexes