2022-11-30, Langbehn, B., Ovcharenko, Y., Clark, A., Coreno, M., Cucini, R., Demidovich, A., Drabbels, M., Finetti, P., Di Fraia, M., Giannessi, L., Grazioli, C., Iablonskyi, D., LaForge, A.C., Nishiyama, T., Oliver Álvarez de Lara, V., Peltz, C., Piseri, P., Plekan, O., Sander, K., Ueda, K., Fennel, T., Prince, K.C., Stienkemeier, F., Callegari, C., Möller, T., Rupp, D.

We explore the light induced dynamics in superfluid helium nanodroplets with wide-angle scattering in a pump–probe measurement scheme. The droplets are doped with xenon atoms to facilitate the ignition of a nanoplasma through irradiation with near-infrared laser pulses. After a variable time delay of up to 800 ps, we image the subsequent dynamics using intense extreme ultraviolet pulses from the FERMI free-electron laser. The recorded scattering images exhibit complex intensity fluctuations that are categorized based on their characteristic features. Systematic simulations of wide-angle diffraction patterns are performed, which can qualitatively explain the observed features by employing model shapes with both randomly distributed as well as structured, symmetric distortions. This points to a connection between the dynamics and the positions of the dopants in the droplets. In particular, the structured fluctuations might be governed by an underlying array of quantized vortices in the superfluid droplet as has been observed in previous small-angle diffraction experiments. Our results provide a basis for further investigations of dopant–droplet interactions and associated heating mechanisms.

2021, Lécz, Zsolt, Andreev, Alexander, Kamperidis, C., Hafz, Nasr

Acceleration of electrons in laser-driven plasma wakefields has been extended up to the ∼8 GeV energy within a distance of tens of centimeters. However, in applications, requiring small energy spread within the electron bunch, only a small portion of the bunch can be used and often the low-energy electrons represent undesired background in the spectrum. We present a compact and tunable scheme providing clean and mono-energetic electron bunches with less than one percent energy spread and with central energy on the GeV level. It is a two-step process consisting of ionization injection with attosecond pulses and acceleration in a capillary plasma wave-guide. Semi-analytical theory and particle-in-cell simulations are used to accurately model the injection and acceleration steps.

2015, Schütte, Bernd, Oelze, Tim, Krikunova, Maria, Arbeiter, Mathias, Fennel, Thomas, Vrakking, Marc J. J., Rouzée, Arnaud

We investigate electron-ion recombination processes in clusters exposed to intense extreme-ultraviolet (XUV) or near-infrared (NIR) pulses. Using the technique of reionization of excited atoms from recombination (REAR), recently introduced in Schütte et al (2014 Phys. Rev. Lett. 112 253401), a large population of excited atoms, which are formed in the nanoplasma during cluster expansion, is identified under both ionization conditions. For intense XUV ionization of clusters, we find that the significance of recombination increases for increasing cluster sizes. In addition, larger fragments are strongly affected by recombination as well, as shown for the case of dimers. We demonstrate that for mixed Ar–Xe clusters exposed to intense NIR pulses, excited atoms and ions are preferentially formed in the Xe core. As a result of electron-ion recombination, higher charge states of Xe are efficiently suppressed, leading to an overall reduced expansion speed of the cluster core in comparison to the shell.

2021, Murillo-Sánchez, Marta L., Reitsma, Geert, Poullain, Sonia Marggi, Fernández-Milán, Pedro, González-Vázquez, Jesús, de Nalda, Rebeca, Martín, Fernando, Vrakking, Marc J. J., Kornilov, Oleg, Bañares, Luis

The time-resolved photodynamics of the methyl iodide cation (CH3I+) are investigated by means of femtosecond XUV-IR pump-probe spectroscopy. A time-delay-compensated XUV monochromator is employed to isolate a specific harmonic, the 9th harmonic of the fundamental 800 nm (13.95 eV, 88.89 nm), which is used as a pump pulse to prepare the cation in several electronic states. A time-delayed IR probe pulse is used to probe the dissociative dynamics on the first excited state potential energy surface. Photoelectrons and photofragment ions - and I+ - are detected by velocity map imaging. The experimental results are complemented with high level ab initio calculations for the potential energy curves of the electronic states of CH3I+ as well as with full dimension on-the-fly trajectory calculations on the first electronically excited state, considering the presence of the IR pulse. The and I+ pump-probe transients reflect the role of the IR pulse in controlling the photodynamics of CH3I+ in the state, mainly through the coupling to the ground state and to the excited state manifold. Oscillatory features are observed and attributed to a vibrational wave packet prepared in the state. The IR probe pulse induces a coupling between electronic states leading to a slow depletion of fragments after the cation is transferred to the ground states and an enhancement of I+ fragments by absorption of IR photons yielding dissociative photoionization. © 2021 The Author(s). Published by IOP Publishing Ltd on behalf of the Institute of Physics and Deutsche Physikalische Gesellschaft.

2015, Richter, Maria, Bouakline, Foudhil, González-Vázquez, Jesús, Martínez-Fernández, Lara, Corral, Inés, Patchkovskii, Serguei, Morales, Felipe, Ivanov, Misha, Martín, Fernando, Smirnova, Olga

Nonadiabatic processes play a fundamental role in the understanding of photochemical processes in excited polyatomic molecules. A particularly important example is that of radiationless electronic relaxation at conical intersections (CIs). We discuss new opportunities for controlling coupled electron–nuclear dynamics at CIs, offered by the advent of nearly single-cycle, phase-stable, mid-infrared laser pulses. To illustrate the control mechanism, a two-dimensional model of the NO2 molecule is considered. The key idea of the control scheme is to match the time scale of the laser field oscillations to the characteristic time scale of the wave packet transit through the CI. The instantaneous laser field changes the shape and position of the CI as the wave packet passes through. As the CI moves in the laser field, it 'slices' through the wave packet, sculpting it in the coordinate and momentum space in a way that is sensitive to the carrier-envelope phase of the control pulse. We find that the electronic coherence imparted on the sub-laser-cycle time scale manifests during much longer nuclear dynamics that follow on the many tens of femtosecond time scale. Control efficiency as a function of molecular orientation is analyzed, showing that modest alignment is sufficient for showing the described effects.

2021, Lécz, Zsolt, Andreev, Alexander, Kamperidis, Christos, Hafz, Nasr

Acceleration of electrons in laser-driven plasma wakefields has been extended up to the 10 GeV energy within a distance of 10s of centimeters. However, in applications, requiring small energy spread within the electron bunch, only a small portion of the bunch can be used and often the low-energy electrons represent undesired background in the spectrum. We present a compact and tunable scheme providing clean and mono-energetic electron bunches with less than one percent energy spread and with central energy on the GeV level. It is a two-step process consisting of ionization injection with attosecond pulses and acceleration in a capillary plasma wave-guide. Semi-analytical theory and particle-in-cell simulations are used to accurately model the injection and acceleration steps.

2015, Brunetti, E., Becker, W., Bryant, H.C., Jaroszynski, D.A., Chou, W.

Direct ionization of hydrogen atoms by laser irradiation is investigated as a potential new scheme to generate proton beams without stripping foils. The time-dependent Schrödinger equation describing the atom-radiation interaction is numerically solved obtaining accurate ionization cross-sections for a broad range of laser wavelengths, durations and energies. Parameters are identified where the Doppler frequency up-shift of radiation colliding with relativistic particles can lead to efficient ionization over large volumes and broad bandwidths using currently available lasers.

2015, Medišauskas, Lukas, Morales, Felipe, Palacios, Alicia, González-Castrillo, Alberto, Plimak, Lev, Smirnova, Olga, Martín, Fernando, Ivanov, Misha Yu

We present an analytical model based on the time-dependent WKB approximation to reproduce the photoionization spectra of an H2 molecule in the autoionization region. We explore the nondissociative channel, which is the major contribution after one-photon absorption, and we focus on the features arising in the energy differential spectra due to the interference between the direct and the autoionization pathways. These features depend on both the timescale of the electronic decay of the autoionizing state and the time evolution of the vibrational wavepacket created in this state. With full ab initio calculations and with a one-dimensional approach that only takes into account the nuclear wavepacket associated to the few relevant electronic states we compare the ground state, the autoionizing state, and the background continuum electronic states. Finally, we illustrate how these features transform from molecular-like to atomic-like by increasing the mass of the system, thus making the electronic decay time shorter than the nuclear wavepacket motion associated with the resonant state. In other words, autoionization then occurs faster than the molecular dissociation into neutrals.